WO2014192708A1 - アクリル樹脂積層フィルム及びその製造方法、並びにメラミン化粧板 - Google Patents
アクリル樹脂積層フィルム及びその製造方法、並びにメラミン化粧板 Download PDFInfo
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- WO2014192708A1 WO2014192708A1 PCT/JP2014/063898 JP2014063898W WO2014192708A1 WO 2014192708 A1 WO2014192708 A1 WO 2014192708A1 JP 2014063898 W JP2014063898 W JP 2014063898W WO 2014192708 A1 WO2014192708 A1 WO 2014192708A1
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- WIPO (PCT)
- Prior art keywords
- acrylic resin
- mass
- laminated film
- parts
- resin composition
- Prior art date
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- 229920000178 Acrylic resin Polymers 0.000 title claims abstract description 265
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- 238000004519 manufacturing process Methods 0.000 title claims description 57
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- 125000001424 substituent group Chemical group 0.000 claims abstract description 51
- 239000000654 additive Substances 0.000 claims abstract description 28
- 230000000996 additive effect Effects 0.000 claims abstract description 26
- -1 methylol group Chemical group 0.000 claims abstract description 21
- 125000003277 amino group Chemical group 0.000 claims abstract description 9
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 33
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- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 23
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- ZGTMUACCHSMWAC-UHFFFAOYSA-L EDTA disodium salt (anhydrous) Chemical compound [Na+].[Na+].OC(=O)CN(CC([O-])=O)CCN(CC(O)=O)CC([O-])=O ZGTMUACCHSMWAC-UHFFFAOYSA-L 0.000 description 4
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- JJBFVQSGPLGDNX-UHFFFAOYSA-N 2-(2-methylprop-2-enoyloxy)propyl 2-methylprop-2-enoate Chemical compound CC(=C)C(=O)OC(C)COC(=O)C(C)=C JJBFVQSGPLGDNX-UHFFFAOYSA-N 0.000 description 1
- GOXQRTZXKQZDDN-UHFFFAOYSA-N 2-Ethylhexyl acrylate Chemical compound CCCCC(CC)COC(=O)C=C GOXQRTZXKQZDDN-UHFFFAOYSA-N 0.000 description 1
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- 229940093475 2-ethoxyethanol Drugs 0.000 description 1
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- IEVADDDOVGMCSI-UHFFFAOYSA-N 2-hydroxybutyl 2-methylprop-2-enoate Chemical compound CCC(O)COC(=O)C(C)=C IEVADDDOVGMCSI-UHFFFAOYSA-N 0.000 description 1
- SCNZQDHXZKQTMA-UHFFFAOYSA-N 2-hydroxyethyl 2-methylprop-2-enoate;styrene Chemical compound C=CC1=CC=CC=C1.CC(=C)C(=O)OCCO SCNZQDHXZKQTMA-UHFFFAOYSA-N 0.000 description 1
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- QTWJRLJHJPIABL-UHFFFAOYSA-N 2-methylphenol;3-methylphenol;4-methylphenol Chemical compound CC1=CC=C(O)C=C1.CC1=CC=CC(O)=C1.CC1=CC=CC=C1O QTWJRLJHJPIABL-UHFFFAOYSA-N 0.000 description 1
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- QZPSOSOOLFHYRR-UHFFFAOYSA-N 3-hydroxypropyl prop-2-enoate Chemical compound OCCCOC(=O)C=C QZPSOSOOLFHYRR-UHFFFAOYSA-N 0.000 description 1
- OFNISBHGPNMTMS-UHFFFAOYSA-N 3-methylideneoxolane-2,5-dione Chemical compound C=C1CC(=O)OC1=O OFNISBHGPNMTMS-UHFFFAOYSA-N 0.000 description 1
- XOJWAAUYNWGQAU-UHFFFAOYSA-N 4-(2-methylprop-2-enoyloxy)butyl 2-methylprop-2-enoate Chemical compound CC(=C)C(=O)OCCCCOC(=O)C(C)=C XOJWAAUYNWGQAU-UHFFFAOYSA-N 0.000 description 1
- OSWFIVFLDKOXQC-UHFFFAOYSA-N 4-(3-methoxyphenyl)aniline Chemical compound COC1=CC=CC(C=2C=CC(N)=CC=2)=C1 OSWFIVFLDKOXQC-UHFFFAOYSA-N 0.000 description 1
- DBCAQXHNJOFNGC-UHFFFAOYSA-N 4-bromo-1,1,1-trifluorobutane Chemical compound FC(F)(F)CCCBr DBCAQXHNJOFNGC-UHFFFAOYSA-N 0.000 description 1
- NDWUBGAGUCISDV-UHFFFAOYSA-N 4-hydroxybutyl prop-2-enoate Chemical compound OCCCCOC(=O)C=C NDWUBGAGUCISDV-UHFFFAOYSA-N 0.000 description 1
- 229920005506 ACRYPET® MD Polymers 0.000 description 1
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- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 description 1
- 229920000298 Cellophane Polymers 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- 239000004606 Fillers/Extenders Substances 0.000 description 1
- CERQOIWHTDAKMF-UHFFFAOYSA-M Methacrylate Chemical compound CC(=C)C([O-])=O CERQOIWHTDAKMF-UHFFFAOYSA-M 0.000 description 1
- NTIZESTWPVYFNL-UHFFFAOYSA-N Methyl isobutyl ketone Chemical compound CC(C)CC(C)=O NTIZESTWPVYFNL-UHFFFAOYSA-N 0.000 description 1
- UIHCLUNTQKBZGK-UHFFFAOYSA-N Methyl isobutyl ketone Natural products CCC(C)C(C)=O UIHCLUNTQKBZGK-UHFFFAOYSA-N 0.000 description 1
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 1
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- 239000004820 Pressure-sensitive adhesive Substances 0.000 description 1
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- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- MBHRHUJRKGNOKX-UHFFFAOYSA-N [(4,6-diamino-1,3,5-triazin-2-yl)amino]methanol Chemical compound NC1=NC(N)=NC(NCO)=N1 MBHRHUJRKGNOKX-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 125000003647 acryloyl group Chemical group O=C([*])C([H])=C([H])[H] 0.000 description 1
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- 150000001338 aliphatic hydrocarbons Chemical class 0.000 description 1
- 125000003342 alkenyl group Chemical group 0.000 description 1
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- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- DIZPMCHEQGEION-UHFFFAOYSA-H aluminium sulfate (anhydrous) Chemical compound [Al+3].[Al+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O DIZPMCHEQGEION-UHFFFAOYSA-H 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 150000008064 anhydrides Chemical class 0.000 description 1
- 125000000129 anionic group Chemical group 0.000 description 1
- 239000003242 anti bacterial agent Substances 0.000 description 1
- 239000002518 antifoaming agent Substances 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 239000008346 aqueous phase Substances 0.000 description 1
- 239000007864 aqueous solution Substances 0.000 description 1
- 239000003125 aqueous solvent Substances 0.000 description 1
- 238000000149 argon plasma sintering Methods 0.000 description 1
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- 229910001628 calcium chloride Inorganic materials 0.000 description 1
- 238000011088 calibration curve Methods 0.000 description 1
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- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 description 1
- NKDDWNXOKDWJAK-UHFFFAOYSA-N dimethoxymethane Chemical compound COCOC NKDDWNXOKDWJAK-UHFFFAOYSA-N 0.000 description 1
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- KCIDZIIHRGYJAE-YGFYJFDDSA-L dipotassium;[(2r,3r,4s,5r,6r)-3,4,5-trihydroxy-6-(hydroxymethyl)oxan-2-yl] phosphate Chemical compound [K+].[K+].OC[C@H]1O[C@H](OP([O-])([O-])=O)[C@H](O)[C@@H](O)[C@H]1O KCIDZIIHRGYJAE-YGFYJFDDSA-L 0.000 description 1
- YHAIUSTWZPMYGG-UHFFFAOYSA-L disodium;2,2-dioctyl-3-sulfobutanedioate Chemical compound [Na+].[Na+].CCCCCCCCC(C([O-])=O)(C(C([O-])=O)S(O)(=O)=O)CCCCCCCC YHAIUSTWZPMYGG-UHFFFAOYSA-L 0.000 description 1
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- STVZJERGLQHEKB-UHFFFAOYSA-N ethylene glycol dimethacrylate Substances CC(=C)C(=O)OCCOC(=O)C(C)=C STVZJERGLQHEKB-UHFFFAOYSA-N 0.000 description 1
- 239000000194 fatty acid Substances 0.000 description 1
- 229930195729 fatty acid Natural products 0.000 description 1
- 150000004665 fatty acids Chemical class 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 239000004088 foaming agent Substances 0.000 description 1
- 235000019253 formic acid Nutrition 0.000 description 1
- 238000010528 free radical solution polymerization reaction Methods 0.000 description 1
- 239000001530 fumaric acid Substances 0.000 description 1
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- 238000005227 gel permeation chromatography Methods 0.000 description 1
- 125000003055 glycidyl group Chemical group C(C1CO1)* 0.000 description 1
- 238000010559 graft polymerization reaction Methods 0.000 description 1
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- 238000007731 hot pressing Methods 0.000 description 1
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- 238000006460 hydrolysis reaction Methods 0.000 description 1
- XLSMFKSTNGKWQX-UHFFFAOYSA-N hydroxyacetone Chemical compound CC(=O)CO XLSMFKSTNGKWQX-UHFFFAOYSA-N 0.000 description 1
- 125000005462 imide group Chemical group 0.000 description 1
- 150000003949 imides Chemical group 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- 238000005342 ion exchange Methods 0.000 description 1
- 239000005453 ketone based solvent Substances 0.000 description 1
- 239000002655 kraft paper Substances 0.000 description 1
- WOFDVDFSGLBFAC-UHFFFAOYSA-N lactonitrile Chemical compound CC(O)C#N WOFDVDFSGLBFAC-UHFFFAOYSA-N 0.000 description 1
- 238000003475 lamination Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- UEGPKNKPLBYCNK-UHFFFAOYSA-L magnesium acetate Chemical compound [Mg+2].CC([O-])=O.CC([O-])=O UEGPKNKPLBYCNK-UHFFFAOYSA-L 0.000 description 1
- 239000011654 magnesium acetate Substances 0.000 description 1
- 235000011285 magnesium acetate Nutrition 0.000 description 1
- 229940069446 magnesium acetate Drugs 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
- 235000019341 magnesium sulphate Nutrition 0.000 description 1
- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 1
- 239000011976 maleic acid Substances 0.000 description 1
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- 230000008018 melting Effects 0.000 description 1
- 150000007522 mineralic acids Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
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- 239000004745 nonwoven fabric Substances 0.000 description 1
- SSDSCDGVMJFTEQ-UHFFFAOYSA-N octadecyl 3-(3,5-ditert-butyl-4-hydroxyphenyl)propanoate Chemical compound CCCCCCCCCCCCCCCCCCOC(=O)CCC1=CC(C(C)(C)C)=C(O)C(C(C)(C)C)=C1 SSDSCDGVMJFTEQ-UHFFFAOYSA-N 0.000 description 1
- KZCOBXFFBQJQHH-UHFFFAOYSA-N octane-1-thiol Chemical compound CCCCCCCCS KZCOBXFFBQJQHH-UHFFFAOYSA-N 0.000 description 1
- ANISOHQJBAQUQP-UHFFFAOYSA-N octyl prop-2-enoate Chemical compound CCCCCCCCOC(=O)C=C ANISOHQJBAQUQP-UHFFFAOYSA-N 0.000 description 1
- 238000007645 offset printing Methods 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 150000007524 organic acids Chemical class 0.000 description 1
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- 239000003960 organic solvent Substances 0.000 description 1
- 239000003973 paint Substances 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 229920001568 phenolic resin Polymers 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 239000004014 plasticizer Substances 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- USHAGKDGDHPEEY-UHFFFAOYSA-L potassium persulfate Chemical compound [K+].[K+].[O-]S(=O)(=O)OOS([O-])(=O)=O USHAGKDGDHPEEY-UHFFFAOYSA-L 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002243 precursor Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- 230000002265 prevention Effects 0.000 description 1
- 235000019260 propionic acid Nutrition 0.000 description 1
- NHARPDSAXCBDDR-UHFFFAOYSA-N propyl 2-methylprop-2-enoate Chemical compound CCCOC(=O)C(C)=C NHARPDSAXCBDDR-UHFFFAOYSA-N 0.000 description 1
- PNXMTCDJUBJHQJ-UHFFFAOYSA-N propyl prop-2-enoate Chemical compound CCCOC(=O)C=C PNXMTCDJUBJHQJ-UHFFFAOYSA-N 0.000 description 1
- LLHKCFNBLRBOGN-UHFFFAOYSA-N propylene glycol methyl ether acetate Chemical group COCC(C)OC(C)=O LLHKCFNBLRBOGN-UHFFFAOYSA-N 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- IUVKMZGDUIUOCP-BTNSXGMBSA-N quinbolone Chemical compound O([C@H]1CC[C@H]2[C@H]3[C@@H]([C@]4(C=CC(=O)C=C4CC3)C)CC[C@@]21C)C1=CCCC1 IUVKMZGDUIUOCP-BTNSXGMBSA-N 0.000 description 1
- 229910001927 ruthenium tetroxide Inorganic materials 0.000 description 1
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- 108700004121 sarkosyl Proteins 0.000 description 1
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- 229940083542 sodium Drugs 0.000 description 1
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- KSAVQLQVUXSOCR-UHFFFAOYSA-M sodium lauroyl sarcosinate Chemical compound [Na+].CCCCCCCCCCCC(=O)N(C)CC([O-])=O KSAVQLQVUXSOCR-UHFFFAOYSA-M 0.000 description 1
- 235000019333 sodium laurylsulphate Nutrition 0.000 description 1
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- RYYKJJJTJZKILX-UHFFFAOYSA-M sodium octadecanoate Chemical compound [Na+].CCCCCCCCCCCCCCCCCC([O-])=O RYYKJJJTJZKILX-UHFFFAOYSA-M 0.000 description 1
- 229940080350 sodium stearate Drugs 0.000 description 1
- JUQGWKYSEXPRGL-UHFFFAOYSA-M sodium;tetradecanoate Chemical compound [Na+].CCCCCCCCCCCCCC([O-])=O JUQGWKYSEXPRGL-UHFFFAOYSA-M 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- KDYFGRWQOYBRFD-UHFFFAOYSA-L succinate(2-) Chemical compound [O-]C(=O)CCC([O-])=O KDYFGRWQOYBRFD-UHFFFAOYSA-L 0.000 description 1
- BDHFUVZGWQCTTF-UHFFFAOYSA-M sulfonate Chemical compound [O-]S(=O)=O BDHFUVZGWQCTTF-UHFFFAOYSA-M 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000006228 supernatant Substances 0.000 description 1
- 230000001629 suppression Effects 0.000 description 1
- 239000002344 surface layer Substances 0.000 description 1
- 238000004381 surface treatment Methods 0.000 description 1
- CIHOLLKRGTVIJN-UHFFFAOYSA-N tert‐butyl hydroperoxide Chemical compound CC(C)(C)OO CIHOLLKRGTVIJN-UHFFFAOYSA-N 0.000 description 1
- 239000002562 thickening agent Substances 0.000 description 1
- 229930192474 thiophene Natural products 0.000 description 1
- 150000004992 toluidines Chemical class 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 239000002759 woven fabric Substances 0.000 description 1
- 229910052724 xenon Inorganic materials 0.000 description 1
- FHNFHKCVQCLJFQ-UHFFFAOYSA-N xenon atom Chemical compound [Xe] FHNFHKCVQCLJFQ-UHFFFAOYSA-N 0.000 description 1
- 239000008096 xylene Substances 0.000 description 1
- 150000007934 α,β-unsaturated carboxylic acids Chemical class 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
- B32B27/308—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising acrylic (co)polymers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
- B29B7/00—Mixing; Kneading
- B29B7/74—Mixing; Kneading using other mixers or combinations of mixers, e.g. of dissimilar mixers ; Plant
- B29B7/7476—Systems, i.e. flow charts or diagrams; Plants
- B29B7/7495—Systems, i.e. flow charts or diagrams; Plants for mixing rubber
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/022—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the choice of material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/03—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the shape of the extruded material at extrusion
- B29C48/07—Flat, e.g. panels
- B29C48/08—Flat, e.g. panels flexible, e.g. films
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/16—Articles comprising two or more components, e.g. co-extruded layers
- B29C48/18—Articles comprising two or more components, e.g. co-extruded layers the components being layers
- B29C48/21—Articles comprising two or more components, e.g. co-extruded layers the components being layers the layers being joined at their surfaces
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C66/00—General aspects of processes or apparatus for joining preformed parts
- B29C66/40—General aspects of joining substantially flat articles, e.g. plates, sheets or web-like materials; Making flat seams in tubular or hollow articles; Joining single elements to substantially flat surfaces
- B29C66/41—Joining substantially flat articles ; Making flat seams in tubular or hollow articles
- B29C66/45—Joining of substantially the whole surface of the articles
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
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Definitions
- the present invention relates to an acrylic resin laminated film, a method for producing the same, and a melamine decorative board.
- Acrylic resin films are excellent in transparency and weather resistance, and have high surface hardness.
- they are bonded to various molded products for indoor or outdoor use, such as optical parts for electrical products, automobile interior parts, signboards, building materials, etc. It is preferably used as a film for protecting the surface.
- surface treatment such as antireflection treatment and antifouling treatment is applied to the surface of the acrylic resin film, and this is bonded to the molded product to give the molded product surface functions such as antireflection and antifouling properties. You can also
- Patent Document 1 discloses a film excellent in adhesiveness containing a polymer containing a monomer having a reactive substituent as a copolymerization component.
- Patent Documents 2 and 3 disclose an acrylic resin film formed of a polymer having a hydroxyl group.
- the objective of this invention is providing the acrylic resin laminated
- the present inventor has found that the object can be achieved by combining two kinds of acrylic resin layers having specific compositions, and has completed the present invention. That is, the present invention relates to the following [1] to [15].
- Acrylic resin layer (I) comprising the acrylic resin composition (A), An acrylic resin laminated film comprising an acrylic resin layer (II) comprising a resin composition (B) containing a reactive group-containing acrylic resin (B-1),
- the resin composition (B) has a total content of 100% by mass of the reactive group-containing acrylic resin (B-1) and the acrylic resin (B-2) other than (B-1) (B- 1) is contained in an amount of 10 to 100% by mass, (B-2) is contained in an amount of 0 to 90% by mass, and (B-1) and (B-2) with respect to a total of 100 parts by mass of (B-1 ) And (B-2) other than additive (C) 0-50 parts by mass
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a reactive substituent for an amino group or a methylol group
- the acrylic resin laminated film whose content rate of the monomer unit which has the said reactive substituent is 3 mass% or more with respect to 100 mass% of the said resin composition (B
- Acrylic resin layer (I) comprising the acrylic resin composition (A), An acrylic resin laminated film comprising an acrylic resin layer (II) comprising a resin composition (B) containing a reactive group-containing acrylic resin (B-1),
- the resin composition (B) has a total content of 100% by mass of the reactive group-containing acrylic resin (B-1) and the acrylic resin (B-2) other than (B-1) (B- 1) is contained in an amount of 10 to 100% by mass, (B-2) is contained in an amount of 0 to 90% by mass, and (B-1) and (B-2) with respect to a total of 100 parts by mass of (B-1 ) And (B-2) other than additive (C) 0-50 parts by mass,
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a hydroxyl group;
- An acrylic resin laminated film, wherein the resin composition (B) has a hydroxyl value of 15 to 300 mgKOH / g.
- the content of the aromatic vinyl monomer unit in the reactive group-containing acrylic resin (B-1) is 0 to 3% by mass with respect to 100% by mass of the resin composition (B).
- [11] A method for producing an acrylic resin laminated film according to any one of [1] to [10], which is produced by a coextrusion method.
- [12] A method for producing an acrylic resin laminated film according to any one of [1] to [10], wherein the acrylic resin laminated film is produced by a coating method.
- an acrylic resin laminated film having excellent bonding properties, water whitening resistance and excellent appearance.
- the acrylic resin laminated film according to the present invention includes an acrylic resin layer (I) made of an acrylic resin composition (A) and an acrylic resin made of a resin composition (B) containing a reactive group-containing acrylic resin (B-1). And a resin layer (II).
- the resin composition (B) constituting the acrylic resin layer (II) has a reactive substituent for expressing adhesiveness with the substrate.
- the acrylic resin layer (II) which consists of a resin composition (B) be a bonding layer toward the to-be-bonded body side, and acrylic resin
- the acrylic resin layer (I) made of the composition (A) is preferably a surface layer facing away from the object to be bonded.
- the acrylic resin composition (A) preferably contains acrylic rubber particles (A-1) from the viewpoint of film productivity and handleability.
- the acrylic rubber particles (A-1) and a thermoplastic polymer ( A-2) and an additive (C) can be contained.
- the acrylic resin composition (A) 5.5 to 100% by mass of (A-1) and (A-2) with respect to 100% by mass of (A-1) and (A-2) in total.
- the additive (C) is preferably contained in an amount of 0 to 20 parts by mass with respect to a total of 100 parts by mass of (A-1) and (A-2). .
- the acrylic resin layer (I) is given more toughness, and the acrylic resin laminated film is less prone to film breakage. It is good. Moreover, the handleability at the time of use of an acrylic resin laminated film is good.
- (A-1) is 10 to 100% by mass and (A-2) is 0 to 0% with respect to 100% by mass in total of (A-1) and (A-2). More preferably, it is 90% by mass, more preferably 15 to 100% by mass of (A-1) and 0 to 85% by mass of (A-2).
- the acrylic resin composition (A) preferably contains 0.1 to 10 parts by mass of the additive (C) with respect to 100 parts by mass in total of (A-1) and (A-2).
- the content is preferably 1 to 8 parts by mass.
- the acrylic resin composition (A) may not contain the thermoplastic polymer (A-2) and the additive (C).
- the acrylic rubber particle (A-1) is not particularly limited as long as it is a particle containing an acrylic resin.
- the acrylic rubber particles (A-1) are two layers in which a layer containing the hard polymer (a-2) as the outer layer is formed on the layer containing the elastic copolymer (a-1) as the inner layer.
- Acrylic rubber particles having the above multilayer structure are preferred.
- the acrylic rubber particle (A-1) is a layer containing an elastic copolymer (a-1) as an inner layer having a structure of one layer or two or more layers obtained mainly from an alkyl (meth) acrylate.
- a layer containing a hard polymer (a-2) as an outer layer having a structure of one layer or two or more layers obtained by graft polymerization of a monomer having an alkyl methacrylate ester as a main component was formed.
- Acrylic rubber particles having a multilayer structure of two or more layers are preferred.
- the acrylic rubber particles (A-1) include an intermediate polymer (a-3) between the layer containing the elastic copolymer (a-1) and the layer containing the hard polymer (a-2). One or more layers may be provided.
- the content of the elastic copolymer (a-1) in the acrylic rubber particles (A-1) is preferably 10 to 90% by mass, more preferably 20 to 70% by mass.
- the content of the hard polymer (a-2) in the acrylic rubber particles (A-1) is preferably 10 to 90% by mass, and more preferably 30 to 70% by mass.
- the content of the intermediate polymer (a-3) in the acrylic rubber particles (A-1) is preferably 0 to 35% by mass, and more preferably 0 to 20% by mass. Moreover, when this content rate is 35 mass% or less, the balance of a final polymer is favorable.
- the elastic copolymer (a-1) is preferably a polymer obtained by polymerizing a monomer composition containing an alkyl (meth) acrylate.
- (meth) acrylic acid shows acrylic acid or methacrylic acid.
- the elastic copolymer (a-1) is more preferably a polymer obtained by polymerizing a monomer composition containing an acrylic acid alkyl ester.
- the monomer composition may further contain a monomer other than (meth) acrylic acid alkyl ester and a crosslinkable monomer.
- the elastic copolymer (a-1) comprises 80 to 100% by mass of an acrylic acid alkyl ester having an alkyl group having 1 to 8 carbon atoms and an alkyl methacrylate having an alkyl group having 1 to 4 carbon atoms ( It can contain 0 to 20% by mass of monomers other than the meth) acrylic acid alkyl ester and 0 to 10% by mass of crosslinkable monomers (100% by mass in total).
- alkyl acrylate ester having an alkyl group having 1 to 8 carbon atoms include methyl acrylate, ethyl acrylate, propyl acrylate, butyl acrylate, 2-ethylhexyl acrylate, and n-octyl acrylate.
- a low acrylic acid alkyl ester is more preferred. These may be used alone or in combination of two or more.
- the alkyl acrylate is used as a main component of the monomer constituting the elastic copolymer (a-1).
- the use amount of the acrylic acid alkyl ester is preferably 30 to 99.9% by mass with respect to all monomers constituting the elastic copolymer (a-1).
- the amount used is 30% by mass or more, the moldability of the film is good.
- the amount used is more preferably 50 to 95% by mass.
- the range of the amount used is the amount of acrylic acid alkyl ester used as a whole of the elastic copolymer (a-1) when the elastic copolymer (a-1) has a structure of two or more layers. Indicates. For example, when the elastic copolymer (a-1) has a hard core structure, the amount of alkyl acrylate ester used in the first layer (core part) can be less than 30% by mass.
- alkyl methacrylate having an alkyl group having 1 to 4 carbon atoms examples include methyl methacrylate, ethyl methacrylate, propyl methacrylate, and butyl methacrylate. These may be used alone or in combination of two or more.
- the amount of methacrylic acid alkyl ester to be used is preferably 0 to 69.9% by mass, more preferably 0 to 40% by mass, based on all monomers constituting the elastic copolymer (a-1).
- Examples of monomers other than (meth) acrylic acid alkyl esters include other vinyl monomers copolymerizable with the above (meth) acrylic acid alkyl esters.
- Examples of monomers other than (meth) acrylic acid alkyl esters include styrene and acrylonitrile. These may be used alone or in combination of two or more.
- the amount used is preferably 0 to 69.9% by mass with respect to all monomers constituting the elastic copolymer (a-1). More preferable is 20% by mass.
- crosslinkable monomer examples include ethylene glycol dimethacrylate, 1,3-butylene glycol dimethacrylate, 1,4-butylene glycol dimethacrylate, propylene glycol dimethacrylate, and a graft crossing agent. These may be used alone or in combination of two or more.
- the amount of the crosslinkable monomer used is preferably from 0.1 to 10% by mass, more preferably from 0.5 to 5% by mass, based on all monomers constituting the elastic copolymer (a-1). From the viewpoint of the stability of the acrylic rubber particles (A-1), it is preferable to use a graft crossing agent as a crosslinkable monomer.
- graft crossing agent examples include allyl ester, methallyl ester or crotyl ester of ⁇ , ⁇ -unsaturated carboxylic acid or unsaturated dicarboxylic acid; triallyl cyanurate, triallyl isocyanurate.
- allyl esters such as acrylic acid, methacrylic acid, maleic acid, and fumaric acid are preferable, and allyl methacrylate is more preferable because it has an excellent effect.
- Such a graft crossing agent mainly has a conjugated unsaturated bond of its ester reacting much faster than an allyl group, a methallyl group or a crotyl group, and chemically bond. And most of the allyl group, methallyl group or crotyl group which reacts slowly works effectively during the polymerization of the next layer polymer to give a graft bond between adjacent two layers.
- the hard polymer (a-2) is preferably a polymer obtained by polymerizing monomers other than methacrylic acid alkyl ester, acrylic acid alkyl ester, and (meth) acrylic acid alkyl ester.
- the hard polymer (a-2) is a methacrylic acid alkyl ester having an alkyl group having 1 to 4 carbon atoms in the presence of the elastic copolymer (a-1), and an alkyl copolymer having 1 to 100% by mass. It is obtained by polymerizing a monomer composed of 0 to 49% by mass of a monomer other than alkyl acrylate having 8 to 8 alkyl groups or a monomer other than (meth) acrylic acid alkyl ester.
- a monomer other than a methacrylic acid alkyl ester having an alkyl group having 1 to 4 carbon atoms, an acrylic acid alkyl ester having an alkyl group having 1 to 8 carbon atoms, and a (meth) acrylic acid alkyl ester may be used as an elastic copolymer.
- a monomer similar to the monomer used for the polymerization of the polymer (a-1) can be used.
- the intermediate polymer (a-3) a monomer composition containing a monomer other than an acrylic acid alkyl ester, a methacrylic acid alkyl ester, a (meth) acrylic acid alkyl ester, and a crosslinkable monomer is polymerized.
- the resulting polymer is preferred.
- the intermediate polymer (a-3) include acrylic acid alkyl esters having an alkyl group having 1 to 8 carbon atoms, methacrylic acid alkyl esters having an alkyl group having 1 to 4 carbon atoms, and (meth) acrylic acid alkyl esters.
- a polymer obtained by polymerizing a monomer composition containing a monomer and a crosslinkable monomer is more preferred.
- the intermediate polymer (a-3) 10 to 90% by mass of an acrylic acid alkyl ester having an alkyl group having 1 to 8 carbon atoms, and 90% of a methacrylic acid alkyl ester having an alkyl group having 1 to 4 carbon atoms.
- a monomer other than (meth) acrylic acid alkyl ester 0 to 10% by mass of a crosslinkable monomer (total 100% by mass).
- the same monomers as those used for the polymerization of the elastic copolymer (a-1) can be used.
- the content (monomer composition ratio) of the acrylic acid alkyl ester in the intermediate polymer (a-3) is lower than the content of the acrylic acid alkyl ester in the elastic copolymer (a-1). It is preferably higher than the content of the alkyl acrylate ester in a-2).
- the average particle diameter of the acrylic rubber particles (A-1) is preferably from 0.01 to 0.5 ⁇ m, more preferably from 0.08 to 0.3 ⁇ m. In particular, from the viewpoint of film formability, the average particle diameter is preferably 0.08 ⁇ m or more.
- the average particle diameter is a value measured by a method described later.
- the method for producing the acrylic rubber particles (A-1) is not particularly limited.
- a method for producing the elastic copolymer (a-1) and the hard polymer (a-2) for example, an emulsion polymerization method can be used. Moreover, it can manufacture also by emulsion suspension polymerization converted into a suspension polymerization system at the time of superposition
- the polymerization temperature is appropriately selected depending on the type and amount of the polymerization initiator used, but is preferably 40 to 120 ° C, more preferably 60 to 95 ° C.
- a known polymerization initiator can be used as the polymerization initiator.
- the polymerization initiator can be added to one or both of the aqueous phase and the monomer phase.
- emulsifiers that can be used in the emulsion polymerization method include anionic, cationic, and nonionic surfactants, with anionic surfactants being preferred.
- Anionic surfactants include, for example, carboxylate surfactants such as potassium oleate, sodium stearate, sodium myristate, sodium N-lauroyl sarcosinate, dipotassium alkenyl succinate; sulfuric acid such as sodium lauryl sulfate Ester salt surfactants; sulfonate surfactants such as sodium dioctyl sulfosuccinate, sodium dodecylbenzenesulfonate, sodium alkyldiphenyl ether disulfonate; phosphate ester surfactants such as sodium polyoxyethylene alkylphenyl ether phosphate Is mentioned. These may be used alone or in combination of two or more.
- the polymer latex obtained by emulsion polymerization can be separated and recovered by a method such as acid coagulation method, salt coagulation method, freeze coagulation method, spray drying method, etc. after filtration through a filter having an opening of 100 ⁇ m or less, for example.
- a method such as acid coagulation method, salt coagulation method, freeze coagulation method, spray drying method, etc. after filtration through a filter having an opening of 100 ⁇ m or less, for example.
- acid coagulation method inorganic acids such as sulfuric acid, hydrochloric acid and phosphoric acid, and organic acids such as acetic acid can be used.
- organic acids such as acetic acid
- inorganic salts such as sodium sulfate, magnesium sulfate, aluminum sulfate and calcium chloride, and organic salts such as calcium acetate and magnesium acetate can be used. These may be used alone or in combination of two or more.
- Acrylic rubber particles (A-1) can be obtained by further washing
- thermoplastic polymer (A-2) is a thermoplastic polymer other than the acrylic rubber particles (A-1), and is preferably a polymer obtained mainly from a methacrylic acid alkyl ester.
- the thermoplastic polymer (A-2) is more preferably a polymer obtained by polymerizing monomers other than methacrylic acid alkyl ester, acrylic acid alkyl ester, and (meth) acrylic acid alkyl ester.
- thermoplastic polymer (A-2) methacrylic acid alkyl ester having an alkyl group having 1 to 4 carbon atoms is 50 to 99.9% by mass, acrylic acid alkyl ester is 0.1 to 50% by mass, and A polymer obtained by polymerizing a total of 100% by mass of 0 to 49.9% by mass of monomers other than (meth) acrylic acid alkyl ester can be used.
- alkyl methacrylate examples include methyl methacrylate, ethyl methacrylate, and butyl methacrylate. Of these, methyl methacrylate is preferred. These may be used alone or in combination of two or more.
- alkyl acrylate ester examples include methyl acrylate, ethyl acrylate, and butyl acrylate. These may be used alone or in combination of two or more.
- Examples of monomers other than (meth) acrylic acid alkyl esters include aromatic vinyl monomers such as styrene, vinyl cyanide monomers such as acrylonitrile, unsaturated dicarboxylic acids such as maleic anhydride and itaconic anhydride.
- aromatic vinyl monomers such as styrene, vinyl cyanide monomers such as acrylonitrile, unsaturated dicarboxylic acids such as maleic anhydride and itaconic anhydride.
- Anhydrides, N-phenylmaleimide and N-cyclohexylmaleimide are mentioned. These may be used alone or in combination of two or more.
- the method for producing the thermoplastic polymer (A-2) is not particularly limited, and various polymerization methods such as suspension polymerization, emulsion polymerization, bulk polymerization and the like can be used. During the polymerization, a chain transfer agent, other polymerization aids, and the like may be used.
- the chain transfer agent is not particularly limited, but mercaptans are preferable.
- the mass average molecular weight of the thermoplastic polymer (A-2) is preferably 300,000 or less from the viewpoint of appropriate elongation during melting of the film raw material resin and good film forming properties.
- the mass average molecular weight is preferably 10,000 or more from the viewpoint that the film does not become brittle and the film breakage hardly occurs during film formation and handling.
- the mass average molecular weight is a value measured by the method described later.
- the additive (C) is a compound other than the acrylic rubber particles (A-1) and the thermoplastic polymer (A-2).
- a stabilizer, a lubricant, a processing aid, a plasticizer, an impact resistance improver examples include foaming agents, fillers, colorants, and ultraviolet absorbers.
- a processing aid is preferable from the viewpoint of ensuring film formability.
- the processing aid is not particularly limited, but a processing aid made of a thermoplastic polymer is preferred, and a polymer obtained by polymerizing methyl methacrylate and a monomer other than methyl methacrylate is more preferred.
- the processing aid for example, a polymer obtained by polymerizing a total of 100% by mass of 50 to 100% by mass of methyl methacrylate and 0 to 50% by mass of monomers other than methyl methacrylate can be used. . Since the film-forming property of the film is improved by using the processing aid, it is effective particularly when the thickness accuracy and the film-forming speed at a high level are required.
- the weight average molecular weight of the processing aid made of a thermoplastic polymer is preferably 400,000 or more, more preferably 500,000 to 5,000,000, and more preferably 700,000 to 500 from the viewpoint of obtaining a film having good thickness accuracy. 2,000,000 is more preferred.
- the mass average molecular weight is a value determined by the method described later.
- Examples of monomers other than methyl methacrylate include alkyl acrylates, alkyl methacrylates other than methyl methacrylate, aromatic vinyl monomers, and vinyl cyanide monomers. These may be used alone or in combination of two or more.
- An emulsion polymerization method is preferred as a method for producing a processing aid comprising a thermoplastic polymer.
- the processing aid made of a thermoplastic polymer can be obtained, for example, by separating and collecting a polymer latex produced by an emulsion polymerization method with various coagulants, or separating and collecting a solid content by spray drying.
- the amount of the processing aid used is preferably 0 to 20 parts by mass with respect to 100 parts by mass in total of the acrylic rubber particles (A-1) and the thermoplastic polymer (A-2).
- this usage-amount is 20 mass parts or less, the viscosity of an acrylic resin composition (A) becomes moderate, and favorable film forming property is obtained.
- the additive (C) is preferably an ultraviolet absorber.
- the molecular weight of the ultraviolet absorber is preferably 300 or more, and more preferably 400 or more. When the molecular weight is 300 or more, the ultraviolet absorber is less likely to volatilize during vacuum molding or pressure molding in an injection mold, and mold contamination is less likely to occur.
- the type of the ultraviolet absorber is not particularly limited, but a benzotriazole ultraviolet absorber having a molecular weight of 400 or more and a triazine ultraviolet absorber having a molecular weight of 400 or more are preferable.
- Examples of commercially available benzotriazole ultraviolet absorbers having a molecular weight of 400 or more include “Tinuvin 234” (trade name, manufactured by Ciba Geigy) and “Adeka Stub LA-31” (trade name, manufactured by ADEKA Corporation).
- As a triazine type ultraviolet absorber having a molecular weight of 400 or more for example, “Tinuvine 1577” (trade name, manufactured by Ciba Geigy) can be mentioned as a commercial product. These may be used alone or in combination of two or more.
- the addition amount of the ultraviolet absorber is preferably 0 to 20 parts by mass with respect to 100 parts by mass in total of the acrylic rubber particles (A-1) and the thermoplastic polymer (A-2) from the viewpoint of weather resistance. 1 to 5 parts by mass is more preferable.
- a radical scavenger such as a hindered amine light stabilizer in combination with the ultraviolet absorber.
- a radical scavenger such as a hindered amine light stabilizer
- commercially available products such as “ADK STAB LA-57”, “ADK STAB LA-62”, “ADK STAB LA-67”, “ADK STAB LA-63”, “ADK STAB LA-68” "Sanol LS-770", “Sanol LS-765", “Sanol LS-292”, “Sanol LS-2626", “Sanol LS-1114", “Sanol LS-” 744 "(all are trade names, manufactured by Sankyo Lifetech Co., Ltd.).
- the addition amount of the radical scavenger is 0 to 10 parts by mass with respect to a total of 100 parts by mass of the acrylic rubber particles (A-1) and the thermoplastic polymer (A-2) from the viewpoint of bleed-out resistance. Is preferable, and 0.2 to 5 parts by mass is more preferable.
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a reactive substituent for the amino group or methylol group, and a resin.
- the content rate of the monomer unit which has a reactive substituent with respect to 100 mass% of compositions (B) is 3 mass% or more.
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a hydroxyl group, and the hydroxyl value of the resin composition (B) is 15-300 mg KOH / g.
- a reactive group-containing acrylic resin (B- 1) By reducing the content of the monomer unit having a reactive substituent in the resin composition and increasing the content of the acrylic resin (B-1) in the resin composition (B), it is possible to improve adhesion and It is possible to achieve both reaction suppression.
- the resin composition (B) can be composed of only the reactive group-containing acrylic resin (B-1) from the viewpoint of productivity.
- the resin composition (B) contains 20 to 100 mass of (B-1) with respect to 100 mass% of the total of (B-1) and (B-2). %, (B-2) is preferably contained in an amount of 0 to 80% by mass, (B-1) is preferably contained in an amount of 40 to 100% by mass, and (B-2) is preferably contained in an amount of 0 to 60% by mass. More preferably, it contains 60 to 100% by mass of B-1) and 0 to 40% by mass of (B-2).
- the resin composition (B) preferably contains 0 to 10 parts by mass of the additive (C) with respect to 100 parts by mass in total of (B-1) and (B-2). The content is more preferably 1 to 5 parts by mass, still more preferably 0.1 to 3 parts by mass.
- the resin composition (B) comprises a reactive group-containing acrylic resin (B-1) and an additive (C), that is, other than (B-1). It is preferable from the viewpoint of productivity that it does not contain the acrylic resin (B-2) and consists only of the reactive group-containing acrylic resin (B-1) and the additive (C).
- the resin composition (B) may not contain the acrylic resin (B-2) and the additive (C) other than (B-1).
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a reactive substituent with respect to an amino group or a methylol group, and the content is 100% of the resin composition (B) 100 It is 3 mass% or more with respect to mass%.
- the monomer unit having a reactive substituent is preferably contained in an amount of 5% by mass or more, and more preferably 10% by mass or more.
- the upper limit of the content rate of the monomer unit which has a reactive substituent is not specifically limited, It can be 50 mass% or less. This content is a value calculated from the amount of raw material charged.
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a hydroxyl group, and the hydroxyl value of the resin composition (B) is 15 to 300 mgKOH / g.
- the hydroxyl value is 15 mgKOH / g or more, good adhesiveness can be obtained.
- the hydroxyl value is 300 mgKOH / g or less, the water absorption of the resin composition (B) is lowered, and the water resistance of the acrylic resin laminated film and the melamine decorative board laminated with the acrylic resin laminated film is improved.
- the hydroxyl value is more preferably 20 to 120 mgKOH / g, still more preferably 25 to 80 mgKOH / g.
- the hydroxyl value is a value calculated by the method described later.
- the glass transition temperature (Tg) of the reactive group-containing acrylic resin (B-1) is preferably 0 to 90 ° C, more preferably 15 to 80 ° C, still more preferably 30 to 75 ° C, and particularly preferably 30 to 70 ° C.
- Tg is 0 ° C. or higher, it is possible to prevent sticking between films at the time of production or handling, and workability is good.
- the heat resistance of the melamine decorative board using the acrylic resin laminated film according to the present invention is good.
- this Tg is 90 degrees C or less, adhesiveness with a melamine base material becomes more favorable.
- the Tg can be obtained from the Fox equation using the Tg value of the homopolymer of the component constituting the reactive group-containing acrylic resin (B-1). The Fox formula is shown below.
- Tg is Tg (° C.) of the copolymer (or a mixture thereof)
- w i is a mass fraction of the monomer i
- Tg i is a Tg of a homopolymer obtained by polymerizing the monomer i. (° C).
- the reactive group-containing acrylic resin (B-1) is not particularly limited as long as it contains a monomer unit having a specific reactive substituent in the above (1) or (2).
- the reactive group-containing acrylic resin (B-1) includes, for example, a monomer unit having a reactive substituent, an aromatic vinyl monomer unit, a monomer unit having a reactive substituent, and an aromatic vinyl monomer. Monomer units other than body units can be contained.
- the reactive group-containing acrylic resin (B-1) is composed of 3 to 100% by mass of monomer units having a reactive substituent, 0 to 3% by mass of aromatic vinyl monomer units, and reactive substitution. A total of 100% by mass of 0 to 97% by mass of monomer units other than the monomer unit having a group and the aromatic vinyl monomer unit can be contained.
- the reactive group-containing acrylic resin (B-1) contains a monomer unit having a reactive substituent for an amino group such as a hydroxyl group or a methylol group
- a material containing methylolmelamine and its derivatives specifically Can be bonded to the melamine decorative board by heating and reacting with the melamine resin of the melamine decorative board or its precursor.
- Examples of the reactive substituent for the amino group or methylol group include a hydroxyl group, a carboxyl group, an amino group, an amide group, an acid anhydride group, an imide group, and an epoxy group.
- the reactive group-containing acrylic resin (B-1) may have one or two or more of these reactive substituents.
- the reaction temperature of the reactive substituent is preferably 50 to 200 ° C., more preferably 110 to 170 ° C., although it varies depending on the presence or absence of a catalyst and the pH value.
- the acrylic resin laminated film according to the present invention is laminated with the melamine base material and heated, Simultaneously with the production of the melamine decorative plate, the acrylic resin laminated film according to the present invention can be sufficiently adhered to the melamine substrate.
- Examples of the monomer having a reactive substituent include a monomer having a hydroxyl group such as (meth) acrylic acid hydroxyalkyl ester; (meth) acrylic acid, (meth) acryloyloxyalkylcarboxylic acid, (meth) acryloyl.
- Monomers having a carboxyl group such as oxyaromatic carboxylic acid
- Monomers having an amino group such as (meth) acrylic acid aminoalkyl ester
- Monomers having an amide group such as (meth) acrylic acid alkylamide alkyl ester
- acid anhydride monomers such as maleic anhydride
- maleimide monomers such as maleimide and alkylmaleimide
- epoxy group-containing contents such as glycidyl (meth) acrylate.
- the monomer having a reactive substituent is a monomer having a hydroxyl group, a carboxyl group, an acid anhydride group, or an epoxy group as a reactive substituent from the viewpoint of adhesiveness.
- the monomer having a reactive substituent is a monomer having a hydroxyl group, a carboxyl group, or an epoxy group as a reactive substituent, and has a hydrolyzable site such as an acid anhydride.
- the monomer having a reactive substituent is more preferably a monomer having a hydroxyl group as a reactive substituent from the viewpoint of preventing crosslinking during melt molding.
- the monomer having a reactive substituent is particularly preferably a monomer having a secondary hydroxyl group as a reactive substituent from the viewpoint of particularly reducing cross-linking during melt molding.
- the monomer having a hydroxyl group as a reactive substituent is preferably hydroxyethyl methacrylate, hydroxypropyl methacrylate, hydroxybutyl methacrylate, hydroxyethyl acrylate, hydroxypropyl acrylate, or hydroxybutyl acrylate.
- hydroxypropyl methacrylate is more preferred as the monomer having a hydroxyl group as a reactive substituent, in that the appearance of the film can be prevented from being poor due to a crosslinking reaction during melt molding.
- the amount of the monomer having a reactive substituent is not particularly limited, but is preferably 3 to 100% by mass with respect to the reactive group-containing acrylic resin (B-1).
- the amount used is more preferably 3 to 80% by mass from the viewpoints of adhesiveness and prevention of side reactions. When the amount used is 3% by mass or more, the adhesiveness becomes better. Moreover, when this usage-amount is 80 mass% or less, the side reaction by a reactive substituent can be suppressed by using 20 mass% or more of a non-reactive monomer together.
- the monomer having a reactive substituent is water-soluble, it is possible to suppress dissolution in water by using a water-insoluble monomer in combination, and efficiency in aqueous polymerization such as emulsion polymerization and suspension polymerization. Thus, a polymer can be produced.
- the amount of the aromatic vinyl monomer used is preferably 0 to 3% by mass with respect to the reactive group-containing acrylic resin (B-1). If this usage-amount is 3 mass% or less, the weather resistance of the acrylic resin laminated film and melamine decorative board obtained will become favorable.
- the amount used is more preferably 0 to 1% by mass, and more preferably 0 to 0.1% by mass.
- the amount used is preferably small, and may be 0% by mass.
- the monomer other than the monomer having a reactive substituent and the aromatic vinyl monomer a monomer similar to the monomer used for the polymerization of the thermoplastic polymer (A-2) may be used.
- an acrylic monomer, particularly methyl methacrylate is preferred.
- the amount of the monomer other than the monomer having the reactive substituent and the aromatic vinyl monomer is selected from the viewpoint of suppressing the reaction such as crosslinking by the reactive substituent. ⁇ 1) is preferably 0 to 97% by mass, more preferably 0 to 90% by mass, and still more preferably 0 to 85% by mass.
- the amount used may be 0% by mass.
- the method for producing the reactive group-containing acrylic resin (B-1) is not particularly limited, and various polymerization methods such as suspension polymerization, emulsion polymerization, bulk polymerization, and solution polymerization can be used. However, when an acid anhydride or a monomer having an imide structure is used as a monomer having a reactive substituent, hydrolysis occurs during the polymerization, and thus it is produced by aqueous polymerization such as suspension polymerization or emulsion polymerization. I can't do it. During the polymerization, a chain transfer agent, other polymerization aids, and the like may be used. The chain transfer agent is not particularly limited, but mercaptans are preferable.
- the acrylic resin (B-2) other than (B-1) is not particularly limited as long as it is an acrylic resin not containing a monomer unit having a reactive substituent.
- an acrylic resin composition (A) As the additive (C), other than the reactive group-containing acrylic resin (B-1) and an acrylic resin (B-2) other than (B-1), an acrylic resin composition (A) can be prepared. The thing similar to the additive (C) to be used can be used.
- the thickness of the acrylic resin laminated film according to the present invention is preferably 100 ⁇ m or less, more preferably 10 to 100 ⁇ m, still more preferably 20 to 75 ⁇ m, and particularly preferably 25 to 60 ⁇ m.
- the thickness is 10 ⁇ m or more, it is easy to produce an acrylic resin laminated film, and sufficient weather resistance can be imparted to the resulting melamine decorative board.
- the thickness is 100 ⁇ m or less, since the acrylic resin laminated film has appropriate flexibility, peeling can be prevented when the resulting melamine decorative board is cut. Further, it is economically advantageous in terms of mass per unit area. Further, the film forming property is stable and the production of the acrylic resin laminated film becomes easy.
- the thickness of the acrylic resin layer (I) is preferably 5 to 99 ⁇ m, more preferably 10 to 55 ⁇ m, and still more preferably 15 to 50 ⁇ m.
- the thickness of the acrylic resin layer (I) is 5 ⁇ m or more, the resulting melamine decorative board has good water resistance.
- the thickness of acrylic resin layer (I) is 99 micrometers or less, it is economically advantageous at the point of the mass per unit area.
- the thickness of the acrylic resin layer (II) is preferably 30 ⁇ m or less, more preferably 1 to 30 ⁇ m, still more preferably 3 to 20 ⁇ m, and particularly preferably 4 to 10 ⁇ m.
- the thickness of the acrylic resin layer (II) is 30 ⁇ m or less, water whitening resistance is improved.
- adhesiveness improves because the thickness of acrylic resin layer (II) is 1 micrometer or more. That is, when the thickness is within these ranges, sufficient water whitening resistance and adhesiveness can be ensured, and an acrylic resin laminated film having a high industrial utility value can be obtained.
- the laminated structure of the acrylic resin layers (I) and (II) is obtained by coextrusion through a feed block die or a multi-manifold die.
- the forming method is preferred.
- the acrylic resin layers (I) and (II) can be formed into a film shape by a melt extrusion method using a T die, and the two types of films can be laminated by a thermal laminating method.
- an extrusion lamination method in which one acrylic resin layer is formed into a film and then the other acrylic resin layer is laminated by a melt extrusion method can be used.
- melt extrusion in order to remove nuclei and impurities that cause surface defects, it is possible to extrude while filtering the resin composition in a molten state with a screen mesh of 200 mesh or more.
- a solution containing the resin composition (B) is applied onto the acrylic resin layer (I) formed into a film shape, and the acrylic resin layer (II ) Is preferably used.
- a solution obtained by dissolving the resin composition (B) in a solvent such as an organic solvent can be obtained by a printing method such as a gravure printing method, a screen printing method, an offset printing method, or a coating method such as a blade coating method or a rod coating method. Examples of the method include coating on the acrylic resin layer (I) and heat drying to remove the solvent.
- the acrylic resin layer (I) may be laminated by applying a solution containing the acrylic resin composition (A) on the acrylic resin layer (II) formed into a film shape.
- the solvent examples include alcohol solvents such as methanol, ethanol, isopropanol, n-butanol and ethylene glycol; aromatic solvents such as xylene, toluene and benzene; aliphatic hydrocarbon solvents such as hexane and pentane; chloroform Halogenated hydrocarbon solvents such as carbon tetrachloride; phenol solvents such as phenol and cresol; ketone solvents such as methyl ethyl ketone, methyl isobutyl ketone, acetone and cyclohexanone; diethyl ether, methoxytoluene, 1,2-dimethoxyethane, Ether solvents such as 1,2-dibutoxyethane, 1,1-dimethoxymethane, 1,1-dimethoxyethane, 1,4-dioxane, tetrahydrofuran (THF); fatty acid solvents such as formic acid, acetic acid,
- Additives for improving solution properties such as anti-skinning agents, thickeners, anti-settling agents, anti-sagging agents, antifoaming agents, leveling agents, etc., depending on the printing suitability or coating suitability as a paint Can be added.
- additives for improving coating film performance such as extender pigments, light stabilizers, ultraviolet absorbers, antioxidants, antibacterial agents, fungicides, and flame retardants can be added to the resin composition.
- the acrylic resin laminated film according to the present invention has excellent adhesiveness and can adhere to various substrates, it can be suitably used as a protective film. That is, the protective film according to the present invention can be composed of the acrylic resin laminated film according to the present invention. In particular, since the acrylic resin laminated film according to the present invention exhibits excellent adhesion to melamine resin, it can be suitably used as a film for protecting the surface of a melamine decorative board. That is, the melamine decorative board surface protecting film according to the present invention can be composed of the acrylic resin laminated film according to the present invention.
- the acrylic resin laminated film according to the present invention and the melamine base material are laminated in the order of the acrylic resin layer (I), the acrylic resin layer (II), and the melamine base material. .
- melamine decorative panels are used on horizontal surfaces such as desks and counters, and vertical surfaces such as walls, and their construction and manufacturing methods are described in detail in the decorative sheet handbook (New Building Materials Research Institute, published in 1973). ing.
- These melamine decorative boards are, for example, impregnating decorative paper for decorative boards with melamine resin, laminating dried melamine resin-impregnated paper and resin-impregnated core paper as a core layer, and if necessary,
- overlay paper is impregnated with melamine resin
- dried melamine resin impregnated overlay paper and balance paper is laminated on the bottom layer for the purpose of suppressing warping, and hot pressing can get.
- a decorative paper for decorative board impregnated with melamine-formaldehyde resin and dried can be used.
- the resin-impregnated core paper include kraft paper, non-woven fabric, woven fabric, etc., a resin liquid mainly composed of phenol-formaldehyde resin, melamine-formaldehyde resin or a mixture thereof, and inorganic such as aluminum hydroxide and calcium carbonate.
- a core paper for a decorative board that has been impregnated with a slurry containing a filler and dried can be used.
- the hot press molding is performed by laminating a resin-impregnated core paper and a melamine resin-impregnated paper (melamine base material) and an acrylic resin laminated film, temperature 110 to 170 ° C., pressure 5 to 10 MPa, time 10 to 90 minutes. It can be done under conditions.
- the acrylic resin layer (II) made of the resin composition (B) is in contact with the melamine base material side and is heat-sealed. It is preferable to make it. According to this method, bonding can be performed without using an adhesive and a pressure-sensitive adhesive. Bonding can be performed continuously or discontinuously, for example, by a non-continuous bonding method using a hot press method.
- the acrylic resin laminated film when producing a melamine decorative board, if the melamine substrate and the acrylic resin laminated film according to the present invention are laminated and hot-press molded, the acrylic resin laminated film can be laminated simultaneously with the production of the melamine decorative board, This is advantageous because the number of steps can be reduced.
- the acrylic resin laminated film according to the present invention when the acrylic resin laminated film according to the present invention is not used, for example, when a film made of the acrylic resin layer (I) is used, the adhesiveness with the melamine base material is low, so the use of an adhesive or a primer is necessary. Yes, the cost is high and productivity is greatly reduced.
- the acrylic resin laminated film according to the present invention when the acrylic resin laminated film according to the present invention is used, since it is not necessary to use an adhesive or a primer, man-hours can be reduced and costs can be reduced, which is industrially advantageous.
- MMA methyl methacrylate MAA: methacrylic acid
- BMA butyl methacrylate MA: methyl acrylate
- BA butyl acrylate
- St styrene
- HEMA 2-hydroxyethyl methacrylate
- HPMA 2-hydroxypropyl methacrylate
- AMA allyl methacrylate
- 1,3BD 1,3-butylene
- CHP cumene hydroperoxide t-BH: t-butyl hydroperoxide t-HH: t-hexyl hydroperoxide
- LPO lauryl peroxide
- n-OM n-octyl mercaptan
- RS-610NA mono-n-dodecyl Sodium oxytetraoxyethylene phosphate (trade name: “Phosphanol RS-610NA”, manufactured by Toho Chemical Industry Co., Ltd.)
- LA-31 “ADEKA STAB LA-31RG” (trade name), manufactured by ADEKA
- Mass average molecular weight (Mw) and molecular weight distribution The mass average molecular weight (Mw) and number average molecular weight of the polymer were determined by the following methods. For samples in which the polymer was dissolved in tetrahydrofuran, gel permeation chromatography (model name: “HLC-8200”, manufactured by Tosoh Corporation), column (trade name: “TSK-GEL SUPER MULTIPIORE HZ-H”, Tosoh Corporation) Using an eluent (tetrahydrofuran), measurement was performed at a temperature of 40 ° C., manufactured by Co., Ltd., inner diameter 4.6 mm ⁇ length 15 cm ⁇ 2 pieces. A mass average molecular weight (Mw) and a number average molecular weight were determined from a calibration curve using standard polystyrene. Furthermore, the molecular weight distribution was calculated by the following formula.
- Glass transition temperature (Tg) It calculated from the formula of FOX using the value as described in the polymer handbook [Polymer HandBook (J. Brandrup, Interscience, 1989)].
- the average particle size of the acrylic rubber particles (A-1) is the final particle size of the polymer latex of the polymer obtained by emulsion polymerization, measured by a light scattering photometer (product name: “DLS-700”). , Manufactured by Otsuka Electronics Co., Ltd.) and measured by a dynamic light scattering method.
- Total light transmittance, haze, yellowness and whiteness was evaluated according to JIS K7361-1, haze value was measured according to JIS K7136, yellowness was evaluated according to JIS K7373, and whiteness was evaluated according to JIS Z8715.
- Adhesion evaluation With respect to the melamine decorative board in the room temperature state, 100 square grids were cut at 1 mm intervals with a cutter knife, and peeling property was confirmed with cellophane tape (manufactured by Nichiban Co., Ltd.). This test was performed before and after the boiling test, and the case where no mass was peeled off was evaluated as ⁇ , the case where 1 to 9 cells were peeled off, and the case where 10 or more cells were peeled off were evaluated as x.
- Acid value (AB) ⁇ f ⁇ 56.1 ⁇ 0.1 / S f: 0.1 mol / L ethanolic potassium hydroxide titer S: Sample amount (g) A: Amount of ethanolic potassium hydroxide used for titration (ml) B: Ethanolic potassium hydroxide amount (ml) used for the blank test.
- the sample was dissolved in acetic anhydride and pyridine, acetylated, and titrated with 0.5 mol / L ethanolic potassium hydroxide solution using phenolphthalein as an indicator. Further, a blank test was carried out by the same operation except that no sample was used, and the hydroxyl value was determined from the following formula.
- Hydroxyl value (BA) ⁇ f ⁇ 56.1 ⁇ 0.5 / S + acid value f: 0.5 mol / L ethanolic potassium hydroxide titer S: sample amount (g) A: Amount of ethanolic potassium hydroxide used for titration (ml) B: Ethanolic potassium hydroxide amount (ml) used for the blank test.
- the value obtained by the above method is taken as the measured value of the hydroxyl value.
- the hydroxyl value in the present invention indicates a measured value of the hydroxyl value.
- the calculated value of the hydroxyl value in Tables 1 and 4 is a value assuming that the introduction rate of the hydroxyl monomer is 100% and the acid value is zero.
- the measured value of the hydroxyl value can be estimated from the calculated value of the hydroxyl value.
- the latex of the acrylic rubber particles (A-1A) was filtered with a filter having an opening of 50 ⁇ m. Next, coagulation, agglomeration and solidification were performed using calcium acetate, filtered, washed with water and dried to obtain acrylic rubber particles (A-1A).
- the raw material (iii) shown below (a part of the raw material for the elastic copolymer (a-1)) was dropped into the polymerization vessel over 90 minutes, and then the reaction was continued for 60 minutes. A latex of coalescence (a-1) was obtained.
- the Tg of the elastic copolymer (a-1) alone was -48 ° C.
- the raw material (iv) shown below was dropped into the polymerization vessel over 45 minutes, and then the reaction was continued for 60 minutes, and the intermediate polymer (a-3) was put on the elastic copolymer (a-1). ) was formed.
- the Tg of the intermediate polymer (a-3) alone was 20 ° C.
- the raw material (v) shown below was dropped into the polymerization vessel over 140 minutes, and then the reaction was continued for 60 minutes, and the hard polymer (a-2) was placed on the intermediate polymer (a-3). Formed.
- a latex containing 100 parts of acrylic rubber particles (A-1B) was obtained.
- the Tg of the hard polymer (a-2) alone was 84 ° C.
- the average particle diameter of the acrylic rubber particles (A-1B) measured after polymerization was 0.12 ⁇ m.
- the latex of the acrylic rubber particles (A-1B) was filtered with a filter having an opening of 50 ⁇ m. Next, coagulation, aggregation, and solidification reaction were performed using calcium acetate, followed by filtration, washing with water, and drying to obtain acrylic rubber particles (A-1B).
- the raw material (iii) shown below (a part of the raw material for the elastic copolymer (a-1)) was dropped into the polymerization vessel over 90 minutes, and then the reaction was continued for 60 minutes. A latex of coalescence (a-1) was obtained.
- the Tg of the elastic copolymer (a-1) alone was ⁇ 20 ° C.
- the raw material (iv) shown below was dropped into the polymerization vessel over 45 minutes, and then the reaction was continued for 60 minutes, and the intermediate polymer (a-3) was put on the elastic copolymer (a-1). ) was formed.
- the Tg of the intermediate polymer (a-3) alone was 60 ° C.
- the raw material (v) shown below was dropped into the polymerization vessel over 140 minutes, and then the reaction was continued for 60 minutes, and the hard polymer (a-2) was placed on the intermediate polymer (a-3). Formed.
- a latex containing 100 parts of acrylic rubber particles (A-1C) was obtained.
- the Tg of the hard polymer (a-2) alone was 99 ° C.
- the average particle diameter of the acrylic rubber particles (A-1C) measured after polymerization was 0.12 ⁇ m.
- the latex of the acrylic rubber particles (A-1C) was filtered through a filter having an opening of 50 ⁇ m. Next, coagulation, aggregation, and solidification reaction were performed using calcium acetate, followed by filtration, washing with water, and drying to obtain acrylic rubber particles (A-1C).
- the mixture was kept for 15 minutes, and the following raw material (iii) (raw material for hard polymer (a-2)) was added while stirring at 80 ° C. in a nitrogen atmosphere. Thereafter, the polymerization was carried out for 1 hour to obtain a latex of acrylic rubber particles (A-1D).
- the average particle diameter of the acrylic rubber particles (A-1D) was 0.12 ⁇ m.
- the latex of the acrylic rubber particles (A-1D) was filtered with a filter having an opening of 50 ⁇ m. Next, coagulation, aggregation and solidification were performed using calcium acetate, filtered, washed with water, and dried to obtain acrylic rubber particles (A-1D).
- the obtained latex was added to a 0.25% by mass aqueous sulfuric acid solution, the polymer was acid coagulated, then dehydrated, washed with water and dried to recover the polymer in powder form.
- the obtained copolymer had a mass average molecular weight of 1,000,000.
- Production of reactive group-containing acrylic resins (B-1A) to (B-1K)> In Production Example 6, the following mixture was charged in a reaction vessel equipped with a stirrer, a reflux condenser, a nitrogen gas inlet, and the like.
- MMA 75 parts BA 10 parts HEMA 15 parts n-OM 0.25 parts LPO 0.4 parts Methyl methacrylate / methacrylate / ethyl methacrylate sulfonate copolymer 0.02 parts Sodium sulfate 0.3 parts Ion exchange 145 parts of water.
- the inside of the container was sufficiently replaced with nitrogen gas, and then heated to 75 ° C. with stirring, and the polymerization reaction was allowed to proceed in a nitrogen gas stream. After 2 hours, the temperature was raised to 95 ° C. and held for another 60 minutes to complete the polymerization. The obtained polymer beads were dehydrated and dried to obtain a reactive group-containing acrylic resin (B-1A).
- a reactive group-containing acrylic resin (B) was prepared in the same manner as in the above procedure except that the raw materials used (MMA, BA, HEMA and n-OH) were changed as shown in Table 1. -1B) to (B-1K) were obtained.
- a dropping solution in which 20 parts of ethyl acetate and 0.6 part of 2,2′-azobis-2-methylbutyronitrile were mixed was added dropwise over 60 minutes and maintained at 95 ° C. for 90 minutes. After cooling this, 200 parts of ethyl acetate was mixed to obtain a resin composition (B23) having a glass transition temperature of 70 ° C. and a weight average molecular weight of 30,000.
- Example 1 Production of acrylic resin laminated film and decorative melamine board>
- the acrylic resin composition (A1) for the acrylic resin layer (I) obtained in Production Example 20 and the resin composition (B1) for the acrylic resin layer (II) obtained in Production Example 28 were 80 ° C. And dried all day and night.
- the resin composition (B1) was plasticized with an extruder of 30 mm ⁇ with the cylinder temperature set to 240 ° C.
- the acrylic resin composition (A1) was plasticized with an extruder of 40 mm ⁇ provided with a 400 mesh screen mesh set at a cylinder temperature of 240 ° C.
- the acrylic resin composition (A1) and the resin composition (B1) are made thick so that the acrylic resin layer (I) side is in contact with the mirror surface cooling roll. It was formed into a 50 ⁇ m acrylic resin laminated film. The thicknesses of the acrylic resin layers (I) and (II) were 45 ⁇ m and 5 ⁇ m, respectively.
- a melamine base material was laminated on the acrylic resin layer (II) surface side of this acrylic resin laminated film, and pressed under conditions of a temperature of 140 ° C., a pressure of 4 MPa, and a time of 20 minutes to produce a melamine decorative board.
- the evaluation results of the obtained melamine decorative board are shown in Table 5 and Table 7.
- the curing temperature of the melamine substrate used was 94 ° C.
- Example 2 to 33 the materials shown in Table 5 were used as the acrylic resin composition (A) for the acrylic resin layer (I) and the resin composition (B) for the acrylic resin layer (II). Then, an acrylic resin laminated film and a melamine decorative board were produced in the same manner as in Example 1 except that the thicknesses of the acrylic resin layers (I) and (II) were as shown in Table 5.
- the evaluation results of the obtained melamine decorative board are shown in Table 5 and Table 7.
- Table 5 the amount of the reactive group-containing acrylic resin (B-1) containing a monomer having a reactive substituent as a copolymerization component with respect to 100% by mass of the resin composition (B) Group content ".
- the functional group content is a value calculated from the amount of raw material charged. The same applies to Table 6.
- Example 34 Preparation of acrylic resin laminated film and melamine decorative board>
- the acrylic resin composition (A4) for the acrylic resin layer (I) obtained in Production Example 23 was dried at 80 ° C. overnight.
- the conditions at that time were a cylinder temperature of 200 to 240 ° C., a T-die temperature of 240 ° C., and a cooling roll temperature of 80 ° C.
- the resin composition (B23) was coated on the 200 mm square acrylic resin film with a bar coater. Then, it was left to stand at 80 degreeC with a warm air dryer for 10 minutes, and the acrylic resin laminated film was obtained by volatilizing a solvent. The thickness of the acrylic resin laminated film was 52 ⁇ m, and the thickness of the acrylic resin layer (II) was 2 ⁇ m.
- a melamine base material was laminated on the acrylic resin layer (II) surface side of this acrylic resin laminated film, and pressed under conditions of a temperature of 140 ° C., a pressure of 4 MPa, and a time of 20 minutes to produce a melamine decorative board.
- Table 6 shows the evaluation results of the obtained melamine decorative board.
- the curing temperature of the melamine substrate used was 94 ° C.
- Example 35 operation of Example 34 except having used the resin composition (B24) instead of the resin composition (B23) as a resin composition (B) for acrylic resin layers (II).
- the resin composition (B24) instead of the resin composition (B23) as a resin composition (B) for acrylic resin layers (II).
- Table 6 shows the evaluation results of the obtained melamine decorative board.
- the acrylic resin laminated films obtained in Examples 1 to 35 are excellent in adhesiveness to melamine substrates, and melamine decorative boards using these acrylic resin laminated films have 10 or more cells peeled off in the adhesion evaluation. There was no. Furthermore, these melamine decorative boards had little change in whiteness after the boiling test, and a remarkable decrease in appearance was suppressed. These acrylic resin laminated films and melamine decorative boards have good adhesiveness and stability against hot water, and have high industrial utility value. In particular, in Examples 1 to 7, 9 to 11, 14, 16, 17, 19 to 21, 23, 24, 28, 29, and 31 to 33, high adhesiveness can be secured even after the boiling test.
- the melamine decorative board using the acrylic resin laminated film is particularly excellent in stability against hot water and has higher industrial utility value.
- the acrylic resin laminated film obtained in Comparative Example 3 has a content of monomer units having a reactive substituent in the resin composition (B) of less than 3% by mass, and the resin composition (B). Has a low hydroxyl value of less than 15 mgKOH / g, the adhesion to the melamine substrate is low, and 10 or more cells were peeled off in the adhesion evaluation.
- this acrylic resin laminated film was used for a melamine decorative board, it peeled off easily, and a melamine decorative board of good quality could not be obtained.
- the acrylic resin laminated film obtained in Comparative Examples 1 and 2 did not have the acrylic resin layer (I) or (II), it was inferior in water resistance, and 10 or more cells were peeled off in the adhesion evaluation.
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Abstract
Description
反応性基含有アクリル樹脂(B-1)を含有する樹脂組成物(B)からなるアクリル樹脂層(II)と、を備えるアクリル樹脂積層フィルムであって、
前記樹脂組成物(B)が、前記反応性基含有アクリル樹脂(B-1)と、(B-1)以外のアクリル樹脂(B-2)との合計100質量%に対して、(B-1)を10~100質量%、(B-2)を0~90質量%含有し、更に、(B-1)と(B-2)との合計100質量部に対して、(B-1)及び(B-2)以外の添加剤(C)を0~50質量部含有し、
前記反応性基含有アクリル樹脂(B-1)がアミノ基又はメチロール基に対する反応性置換基を有する単量体単位を含有し、
前記反応性置換基を有する単量体単位の含有率が、前記樹脂組成物(B)100質量%に対して3質量%以上である、アクリル樹脂積層フィルム。
反応性基含有アクリル樹脂(B-1)を含有する樹脂組成物(B)からなるアクリル樹脂層(II)と、を備えるアクリル樹脂積層フィルムであって、
前記樹脂組成物(B)が、前記反応性基含有アクリル樹脂(B-1)と、(B-1)以外のアクリル樹脂(B-2)との合計100質量%に対して、(B-1)を10~100質量%、(B-2)を0~90質量%含有し、更に、(B-1)と(B-2)との合計100質量部に対して、(B-1)及び(B-2)以外の添加剤(C)を0~50質量部含有し、
前記反応性基含有アクリル樹脂(B-1)が水酸基を有する単量体単位を含有し、
前記樹脂組成物(B)の水酸基価が15~300mgKOH/gである、アクリル樹脂積層フィルム。
本発明に係るアクリル樹脂積層フィルムは、アクリル樹脂組成物(A)からなるアクリル樹脂層(I)と、反応性基含有アクリル樹脂(B-1)を含有する樹脂組成物(B)からなるアクリル樹脂層(II)とを備える。ここで、アクリル樹脂層(II)を構成する樹脂組成物(B)は、基材との接着性を発現するための反応性置換基を有している。このため、本発明に係るアクリル樹脂積層フィルムを貼合用途に用いる場合には、樹脂組成物(B)からなるアクリル樹脂層(II)を被貼合体側に向けて貼合層とし、アクリル樹脂組成物(A)からなるアクリル樹脂層(I)を被貼合体とは反対側に向けて表面層とするのが好ましい。
まず、アクリル樹脂層(I)を構成するアクリル樹脂組成物(A)について説明する。
アクリルゴム粒子(A-1)は、アクリル樹脂を含む粒子であれば特に限定されない。しかしながら、アクリルゴム粒子(A-1)は、内層としての弾性共重合体(a-1)を含む層上に、外層としての硬質重合体(a-2)を含む層が形成された2層以上の多層構造を有するアクリルゴム粒子であることが好ましい。
熱可塑性重合体(A-2)は、アクリルゴム粒子(A-1)以外の熱可塑性重合体であり、メタクリル酸アルキルエステルを主成分として得られる重合体であることが好ましい。熱可塑性重合体(A-2)としては、メタクリル酸アルキルエステル、アクリル酸アルキルエステル、及び、(メタ)アクリル酸アルキルエステル以外の単量体を重合して得られる重合体がより好ましい。例えば、熱可塑性重合体(A-2)としては、炭素数1~4のアルキル基を有するメタクリル酸アルキルエステル50~99.9質量%、アクリル酸アルキルエステル0.1~50質量%、及び、(メタ)アクリル酸アルキルエステル以外の単量体0~49.9質量%の合計100質量%を重合して得られる重合体を用いることができる。
添加剤(C)は、アクリルゴム粒子(A-1)及び熱可塑性重合体(A-2)以外の化合物であり、例えば、安定剤、滑剤、加工助剤、可塑剤、耐衝撃向上剤、発泡剤、充填剤、着色剤、紫外線吸収剤が挙げられる。
次に、アクリル樹脂層(II)を構成する樹脂組成物(B)について説明する。樹脂組成物(B)は、以下の(1)又は(2)で表現される。
式中、Tgは共重合体(または、その混合物)のTg(℃)、wiは単量体iの質量分率、Tgiは単量体iを重合して得られる単独重合体のTg(℃)である。
反応性基含有アクリル樹脂(B-1)は、前記(1)又は(2)における特定の反応性置換基を有する単量体単位を含有すれば、特に限定されない。反応性基含有アクリル樹脂(B-1)は、例えば、反応性置換基を有する単量体単位、芳香族ビニル単量体単位、反応性置換基を有する単量体単位及び芳香族ビニル単量体単位以外の単量体単位を含有することができる。具体的には、反応性基含有アクリル樹脂(B-1)は、反応性置換基を有する単量体単位3~100質量%、芳香族ビニル単量体単位0~3質量%、反応性置換基を有する単量体単位及び芳香族ビニル単量体単位以外の単量体単位0~97質量%の合計100質量%を含有することができる。
(B-1)以外のアクリル樹脂(B-2)は、反応性置換基を有する単量体単位を含有しないアクリル樹脂であれば、特に限定されない。(B-1)以外のアクリル樹脂(B-2)の構造、使用される単量体、製造方法、各種物性としては、前記アクリルゴム粒子(A-1)又は前記熱可塑性重合体(A-2)と同様である。
添加剤(C)としては、反応性基含有アクリル樹脂(B-1)、及び(B-1)以外のアクリル樹脂(B-2)以外であれば、アクリル樹脂組成物(A)の調製に用いる添加剤(C)と同様のものを用いることができる。
本発明に係るアクリル樹脂積層フィルムは優れた接着性を有し、各種の基材に接着することができるため、保護フィルムとして好適に使用できる。即ち、本発明に係る保護フィルムは、本発明に係るアクリル樹脂積層フィルムからなることができる。特に、本発明に係るアクリル樹脂積層フィルムはメラミン樹脂に対して優れた接着性を示すため、メラミン化粧板表面保護用フィルムとして好適に使用できる。即ち、本発明に係るメラミン化粧板表面保護用フィルムは、本発明に係るアクリル樹脂積層フィルムからなることができる。また、本発明に係るメラミン化粧板は、本発明に係るアクリル樹脂積層フィルムと、メラミン基材とが、アクリル樹脂層(I)、アクリル樹脂層(II)、メラミン基材の順に積層されている。
MAA:メタクリル酸
BMA:ブチルメタクリレート
MA:メチルアクリレート
BA:ブチルアクリレート
St:スチレン
HEMA:2-ヒドロキシエチルメタクリレート
HPMA:2-ヒドロキシプロピルメタクリレート
AMA:アリルメタクリレート
1,3BD:1,3-ブチレングリコールジメタクリレート
CHP:クメンヒドロペルオキシド
t-BH:t-ブチルハイドロパーオキサイド
t-HH:t-ヘキシルハイドロパーオキサイド
LPO:ラウリルパーオキサイド
n-OM:n-オクチルメルカプタン
RS-610NA:モノ-n-ドデシルオキシテトラオキシエチレン燐酸ナトリウム(商品名:「フォスファノールRS-610NA」、東邦化学工業(株)製)
LA-31:(株)ADEKA製、「アデカスタブLA-31RG」(商品名)
LA-57:(株)ADEKA製、「アデカスタブLA-57」(商品名)
TV234:BASF製、「Tinuvin234」(商品名)
TV1600:BASF製、「Tinuvin1600」(商品名)
Irg1076:BASF製、「Irganox1076」(商品名)
VH:三菱レイヨン(株)製、「アクリペットVH」(商品名)
MD:三菱レイヨン(株)製、「アクリペットMD」(商品名)。
重合体の質量平均分子量(Mw)及び数平均分子量を、以下の方法により求めた。重合体をテトラヒドロフランに溶解させた試料について、ゲルパーミエーションクロマトグラフィー(機種名:「HLC-8200」、東ソー(株)製)、カラム(商品名:「TSK-GEL SUPER MULTIPORE HZ-H」、東ソー(株)製、内径4.6mm×長さ15cm×2本)、溶離液(テトラヒドロフラン)を用いて、温度40℃で測定を行なった。標準ポリスチレンによる検量線から、質量平均分子量(Mw)及び数平均分子量を求めた。更に、下記式により分子量分布を算出した。
ポリマーハンドブック[Polymer HandBook(J.Brandrup,Interscience,1989)]に記載されている値を用いてFOXの式から算出した。
アクリルゴム粒子(A-1)の平均粒子径は、乳化重合で得られた重合体のポリマーラテックスの最終粒子径を、光散乱光度計(製品名:「DLS-700」、大塚電子(株)製)を用い、動的光散乱法で測定した。
フィルム状に成形する前のアクリル樹脂ペレットを、クロロホルムに溶解させて1質量%クロロホルム溶液を調製し、25℃にて一昼夜放置した。その後、これに対し16000r.p.m.で90分間遠心分離を施し、その上澄み液を除き、乾燥した後の不溶分の質量%をゲル含有率とした。
全光線透過率はJIS K7361-1、曇価はJIS K7136、黄色度はJIS K7373、白度はJIS Z8715に準拠して評価した。
DSC6200(製品名、SIIナノテクノロジー製)を用いて、メラミン基材を窒素気流下、25℃から200℃まで10℃/分で昇温した際の吸熱ピーク温度を測定して、メラミン基材硬化温度とした。
CEN(欧州標準化委員会)規格、EN438-2に従い、100℃、2時間煮沸試験を実施し、煮沸試験前後の白度変化を測定した。
室温状態のメラミン化粧板に対し、カッターナイフにより1mm間隔で100マスの碁盤目の切り込みを入れ、セロハンテープ(ニチバン(株)製)で剥がれ性を確認した。この試験を前記煮沸試験前後に行ない、マスが全く剥がれない場合を○、1個以上9個以下のマスが剥がれる場合を△、10個以上のマスが剥がれる場合を×と評価した。
アクリル樹脂積層フィルムを適当な大きさに切り出し、切片を0.5質量%四酸化ルテニウム水溶液に、室温で15時間浸漬して染色した。更に、ミクロトームを用いて断面層が観察できるように、約70nmの厚さに試料を切断し、透過型電子顕微鏡で断面層を写真撮影した。この写真からアクリルゴム粒子(A-1)が存在しない部分の厚さを求めて、アクリル樹脂層(II)の厚さとした。
スーパーキセノンウェザーメーター SX75(商品名、スガ試験機(株)製)を用い、照射強度60W/m2(300~400nm)、フィルター#275にて、照射(63℃、50%RH)102分、照射+噴霧(95%RH)18分の、計120分を1サイクルとして、メラミン化粧板に対して試験を実施した。試験前後での密着性と白度を、上記と同様に評価した。
まず、以下の方法によりサンプルの酸価を求めた。サンプルをアセトンに溶解し、フェノールフタレインを指示薬として、0.1mol/Lのエタノール性水酸化カリウム溶液で滴定した。また、サンプルを使用しない他は同様の操作で空試験を実施し、以下の式から酸価を求めた。
f:0.1mol/Lエタノール性水酸化カリウムの力価
S:サンプル量(g)
A:滴定に用いたエタノール性水酸化カリウム量(ml)
B:空試験に用いたエタノール性水酸化カリウム量(ml)。
f:0.5mol/Lエタノール性水酸化カリウムの力価
S:サンプル量(g)
A:滴定に用いたエタノール性水酸化カリウム量(ml)
B:空試験に用いたエタノール性水酸化カリウム量(ml)。
目視にてフィルム外観を観察し、100cm2あたりの異物数を計数した。
○:0~1個/100cm2
△:2~10個/100cm2。
JIS K5600-5-4に準拠し評価した。
窒素雰囲気下、還流冷却器付き反応容器に脱イオン水206部を入れ、80℃に昇温した。以下に示す成分(i)を添加し、撹拌を行ないながら以下に示す原料(ii)(弾性共重合体(a-1)用原料の一部)の1/10を仕込み、15分保持した。次いで、残りの原料(ii)を、水に対する単量体混合物の増加率が8質量%/時間となるように連続的に添加した。その後1時間保持して重合を行ない、重合体ラテックスを得た。続いて、該重合体ラテックスにソジウムホルムアルデヒドスルホキシレート0.2部を加えた。その後15分保持し、窒素雰囲気下80℃で撹拌を行ないながら、以下に示す原料(iii)(弾性共重合体(a-1)用原料の一部)を、水に対する単量体混合物の増加率が4質量%/時間となるように連続的に添加した。その後2時間保持して重合を行ない、弾性共重合体(a-1)のラテックスを得た。
ソジウムホルムアルデヒドスルホキシレート 0.4部
硫酸第一鉄 0.00004部
エチレンジアミン四酢酸二ナトリウム 0.00012部
(ii)
MMA 11.25部
BA 12.5部
St 1.25部
AMA 0.094部
1,3BD 0.75部
t-BH 0.044部
RS-610NA 0.75部
(iii)
BA 30.9部
St 6.6部
AMA 0.66部
1,3BD 0.09部
CHP 0.11部
RS-610NA 0.6部
(iv)
MMA 35.6部
MA 1.9部
n-OM 0.11部
t-BH 0.06部。
攪拌機を備えた容器に脱イオン水8.5部を仕込んだ後、撹拌を行ないながら以下に示す原料(ii)(弾性共重合体(a-1)用原料の一部)を加え、20分間攪拌を実施して乳化液を調製した。
ソジウムホルムアルデヒドスルホキシレート 0.2部
硫酸第一鉄 0.0001部
エチレンジアミン四酢酸二ナトリウム 0.0003部
(ii)
MMA 0.3部
BA 4.5部
AMA 0.05部
1,3BD 0.2部
CHP 0.025部
RS-610NA 1.1部
(iii)
MMA 1.5部
BA 22.5部
AMA 0.25部
1,3BD 1.0部
CHP 0.016部
(iv)
MMA 6.0部
BA 4.0部
AMA 0.075部
CHP 0.013部
(v)
MMA 55.2部
BA 4.8部
n-OM 0.22部
t-BH 0.075部。
攪拌機を備えた容器に脱イオン水8.5部を仕込んだ後、撹拌を行ないながら以下に示す原料(ii)(弾性共重合体(a-1)用原料の一部)を加え、20分間攪拌を実施して乳化液を調製した。
ソジウムホルムアルデヒドスルホキシレート 0.2部
硫酸第一鉄 0.0001部
エチレンジアミン四酢酸二ナトリウム 0.0003部
(ii)
MMA 0.3部
BA 4.5部
AMA 0.05部
1,3BD 0.2部
CHP 0.025部
RS-610NA 1.3部
(iii)
MMA 9.6部
BA 14.4部
AMA 0.25部
1,3BD 1.0部
CHP 0.016部
(iv)
MMA 6.0部
MA 4.0部
AMA 0.075部
CHP 0.013部
(v)
MMA 57部
MA 3部
n-OM 0.26部
t-BH 0.075部。
窒素雰囲気下、還流冷却器付き反応容器に脱イオン水153部を入れ、80℃に昇温した。以下に示す成分(i)を添加し、撹拌を行ないながら以下に示す原料(ii)(弾性共重合体(a-1)用原料)を添加した。その後1時間保持して重合を行ない、重合体ラテックスを得た。続いて、該重合体ラテックスにソジウムホルムアルデヒドスルホキシレート0.1部を加えた。その後15分保持し、窒素雰囲気下80℃で撹拌を行ないながら、以下に示す原料(iii)(硬質重合体(a-2)用原料)を添加した。その後1時間保持して重合を行ない、アクリルゴム粒子(A-1D)のラテックスを得た。アクリルゴム粒子(A-1D)の平均粒子径は0.12μmであった。
ソジウムホルムアルデヒドスルホキシレート 0.4部
硫酸第一鉄 0.00004部
エチレンジアミン四酢酸二ナトリウム 0.00012部
(ii)
BA 50.9部
St 11.6部
AMA 0.56部
t-BH 0.19部
RS-610NA 1.0部
(iii)
MMA 35.6部
MA 1.9部
t-BH 0.056部
n-OM 0.16部
RS-610NA 0.25部。
反応容器内に窒素置換したイオン交換水200部を仕込み、乳化剤としてオレイン酸カリウム1部、過硫酸カリウム0.3部を仕込んだ。続いてMMA40部、BA10部、n-OM0.005部を仕込み、窒素雰囲気下65℃にて3時間撹拌し、重合を完結させた。引き続いて、MMA48部及びBA2部からなる単量体混合物を2時間にわたり滴下し、滴下終了後2時間保持し、重合を完結させた。得られたラテックスを0.25質量%硫酸水溶液に添加し、重合体を酸凝析し、その後脱水、水洗、乾燥し、粉体状で重合体を回収した。得られた共重合体の質量平均分子量は1,000,000であった。
製造例6では、撹拌機、還流冷却器、及び窒素ガス導入口等の付いた反応容器内に、以下の混合物を仕込んだ。
BA 10部
HEMA 15部
n-OM 0.25部
LPO 0.4部
メチルメタクリレート/メタクリル酸塩/メタクリル酸エチルスルホン酸塩の共重合体 0.02部
硫酸ナトリウム 0.3部
イオン交換水 145部。
製造例2における原料(v)のうち、MMA及びBA(計60部)に代えて、表2に示す通りの原料を使用した以外は、製造例2と同様にして、反応性基含有アクリル樹脂(B-1L)~(B-1N)を得た。
製造例20では、アクリルゴム粒子(A-1)として、製造例1のアクリルゴム粒子(A-1A)16部と、熱可塑性重合体(A-2)であるVH84部とを混合した重合体混合物100部に対し、製造例5の熱可塑性重合体(C1)を1部、LA-31を2部、LA-57を0.1部、Irg1076を0.1部加え、ヘンシェルミキサーを用いて混合した。次いで、これを35mmφのスクリュー型2軸押出機(L/D=26)を用いて、シリンダー温度200℃~240℃、ダイ温度240℃の条件下で溶融混練し、ペレット化して、アクリル樹脂層(I)用のアクリル樹脂組成物(A1)を得た。
製造例28では、反応性基含有アクリル樹脂(B-1)として、製造例5の反応性基含有アクリル樹脂(B-1A)を100部、Irg1076を0.1部用い、これらをヘンシェルミキサーで混合した。次いで、これを35mmφのスクリュー型2軸押出機(L/D=26)を用いて、シリンダー温度200℃~240℃、ダイ温度240℃の条件下で溶融混練し、ペレット化して、アクリル樹脂層(II)用の樹脂組成物(B1)を得た。
窒素導入口、攪拌機、コンデンサー、滴下漏斗、及び温度計を備えたフラスコに、窒素雰囲気下で、酢酸i-ブチルを47部、酢酸エチルを18部入れた。フラスコ内を攪拌しながら内温を95℃に上げた。その後、下記単量体混合物を滴下漏斗より3時間かけてフラスコ内に滴下し、95℃で1時間保持した。
MAA 0.3部
MMA 22.7部
St 30部
BMA 21部
HEMA 26部
2,2’-アゾビス-2-メチルブチロニトリル 0.7部
酢酸エチル 10部。
前記樹脂組成物(B23)100部に、アクリルゴム粒子(A-1B)を22.5部、酢酸エチルを260部混ぜて、樹脂組成物(B24)を得た。
実施例1では、製造例20で得たアクリル樹脂層(I)用のアクリル樹脂組成物(A1)、製造例28で得たアクリル樹脂層(II)用の樹脂組成物(B1)を80℃で一昼夜乾燥した。シリンダー温度を240℃に設定した30mmφの押出し機で樹脂組成物(B1)を可塑化した。また、シリンダー温度を240℃に設定した400メッシュのスクリーンメッシュを設けた40mmφの押出し機でアクリル樹脂組成物(A1)を可塑化した。次いで、250℃に設定した2種2層用フィードブロックダイで、アクリル樹脂層(I)側が鏡面冷却ロールに接するようにして、アクリル樹脂組成物(A1)及び樹脂組成物(B1)を厚さ50μmのアクリル樹脂積層フィルムに製膜した。アクリル樹脂層(I)及び(II)の厚さはそれぞれ45μm及び5μmであった。
実施例34では、製造例23で得たアクリル樹脂層(I)用のアクリル樹脂組成物(A4)を80℃で一昼夜乾燥した。この乾燥ペレットを、300mm幅のTダイを取り付けた40mmφのノンベントスクリュー型押出機(L/D=26)に供給して、厚さ50μmのアクリル樹脂フィルムを作製した。その際の条件は、シリンダー温度が200~240℃、Tダイ温度が240℃、冷却ロール温度が80℃であった。
アクリル樹脂層(I)用のアクリル樹脂組成物(A)、アクリル樹脂層(II)用の樹脂組成物(B)として、表5に示す通りの材料を使用し、アクリル樹脂層(I)及び(II)の厚さを表5に示す通りとしたこと以外は、実施例1と同様にして、アクリル樹脂積層フィルム及びメラミン化粧板を作製した。得られたメラミン化粧板の評価結果を表5、表7に示す。(I)層又は(II)層の記載がないものは単層のフィルムである。
Claims (15)
- アクリル樹脂組成物(A)からなるアクリル樹脂層(I)と、
反応性基含有アクリル樹脂(B-1)を含有する樹脂組成物(B)からなるアクリル樹脂層(II)と、を備えるアクリル樹脂積層フィルムであって、
前記樹脂組成物(B)が、前記反応性基含有アクリル樹脂(B-1)と、(B-1)以外のアクリル樹脂(B-2)との合計100質量%に対して、(B-1)を10~100質量%、(B-2)を0~90質量%含有し、更に、(B-1)と(B-2)との合計100質量部に対して、(B-1)及び(B-2)以外の添加剤(C)を0~50質量部含有し、
前記反応性基含有アクリル樹脂(B-1)がアミノ基又はメチロール基に対する反応性置換基を有する単量体単位を含有し、
前記反応性置換基を有する単量体単位の含有率が、前記樹脂組成物(B)100質量%に対して3質量%以上である、アクリル樹脂積層フィルム。 - 前記反応性置換基が水酸基である、請求項1に記載のアクリル樹脂積層フィルム。
- 前記反応性置換基が2級水酸基である、請求項1に記載のアクリル樹脂積層フィルム。
- アクリル樹脂組成物(A)からなるアクリル樹脂層(I)と、
反応性基含有アクリル樹脂(B-1)を含有する樹脂組成物(B)からなるアクリル樹脂層(II)と、を備えるアクリル樹脂積層フィルムであって、
前記樹脂組成物(B)が、前記反応性基含有アクリル樹脂(B-1)と、(B-1)以外のアクリル樹脂(B-2)との合計100質量%に対して、(B-1)を10~100質量%、(B-2)を0~90質量%含有し、更に、(B-1)と(B-2)との合計100質量部に対して、(B-1)及び(B-2)以外の添加剤(C)を0~50質量部含有し、
前記反応性基含有アクリル樹脂(B-1)が水酸基を有する単量体単位を含有し、
前記樹脂組成物(B)の水酸基価が15~300mgKOH/gである、アクリル樹脂積層フィルム。 - 前記アクリル樹脂組成物(A)がアクリルゴム粒子(A-1)を含有する、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 前記反応性基含有アクリル樹脂(B-1)のガラス転移温度が0~90℃である、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 前記反応性基含有アクリル樹脂(B-1)中の芳香族ビニル単量体単位の含有率が、前記反応性基含有アクリル樹脂(B-1)100質量%に対して0~3質量%である、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 前記樹脂組成物(B)が、前記反応性基含有アクリル樹脂(B-1)及び前記添加剤(C)からなる、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 厚さが100μm以下である、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 前記アクリル樹脂層(II)の厚さが30μm以下である、請求項1又は4に記載のアクリル樹脂積層フィルム。
- 請求項1又は4に記載のアクリル樹脂積層フィルムの製造方法であって、共押出法により製造する、アクリル樹脂積層フィルムの製造方法。
- 請求項1又は4に記載のアクリル樹脂積層フィルムの製造方法であって、塗工法により製造する、アクリル樹脂積層フィルムの製造方法。
- 請求項1又は4に記載のアクリル樹脂積層フィルムの、保護フィルムとしての使用。
- 請求項1又は4に記載のアクリル樹脂積層フィルムの、メラミン化粧板表面保護用フィルムとしての使用。
- 請求項1又は4に記載のアクリル樹脂積層フィルムと、メラミン基材とが、アクリル樹脂層(I)、アクリル樹脂層(II)、メラミン基材の順に積層されたメラミン化粧板。
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US14/894,009 US10562283B2 (en) | 2013-05-27 | 2014-05-27 | Acrylic resin laminate film, manufacturing method therefor, and melamine decorative board |
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JP2014527390A JP6413765B2 (ja) | 2013-05-27 | 2014-05-27 | アクリル樹脂積層フィルム及びその製造方法、並びにメラミン化粧板 |
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US11958994B2 (en) | 2019-03-29 | 2024-04-16 | Dai Nippon Printing Co., Ltd. | Sheet, ornamental material, and resin composition |
JP7509136B2 (ja) | 2019-03-29 | 2024-07-02 | 大日本印刷株式会社 | 化粧シート、化粧材及び樹脂組成物 |
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EP3398772B1 (en) * | 2014-11-26 | 2020-04-29 | Mitsubishi Chemical Corporation | Resin laminate film, method for manufacturing same, and melamine decorative panel |
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US11958994B2 (en) | 2019-03-29 | 2024-04-16 | Dai Nippon Printing Co., Ltd. | Sheet, ornamental material, and resin composition |
JP7509136B2 (ja) | 2019-03-29 | 2024-07-02 | 大日本印刷株式会社 | 化粧シート、化粧材及び樹脂組成物 |
WO2023042922A1 (ja) | 2021-09-17 | 2023-03-23 | 三菱ケミカル株式会社 | 多層フィルムの製造方法、メラミン化粧板の製造方法、多層フィルム、メラミン化粧板用保護フィルム、及びメラミン化粧板 |
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EP3006208A1 (en) | 2016-04-13 |
CN105307862B (zh) | 2017-05-10 |
KR101870499B1 (ko) | 2018-06-22 |
JP6413765B2 (ja) | 2018-10-31 |
KR20160003791A (ko) | 2016-01-11 |
US20160107428A1 (en) | 2016-04-21 |
US10562283B2 (en) | 2020-02-18 |
JPWO2014192708A1 (ja) | 2017-02-23 |
EP3006208A4 (en) | 2016-04-13 |
CN105307862A (zh) | 2016-02-03 |
EP3006208B1 (en) | 2022-06-29 |
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