JP6829685B2 - Heat storage material composition, heat storage molded body, heat storage building material, heat storage building material board, and heat storage plaster wall material - Google Patents
Heat storage material composition, heat storage molded body, heat storage building material, heat storage building material board, and heat storage plaster wall material Download PDFInfo
- Publication number
- JP6829685B2 JP6829685B2 JP2017528650A JP2017528650A JP6829685B2 JP 6829685 B2 JP6829685 B2 JP 6829685B2 JP 2017528650 A JP2017528650 A JP 2017528650A JP 2017528650 A JP2017528650 A JP 2017528650A JP 6829685 B2 JP6829685 B2 JP 6829685B2
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- JP
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- Prior art keywords
- heat storage
- thermoplastic elastomer
- mass
- mineral oil
- vegetable oil
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 239000000203 mixture Substances 0.000 title claims description 102
- 238000005338 heat storage Methods 0.000 title claims description 57
- 239000011232 storage material Substances 0.000 title claims description 32
- 239000004566 building material Substances 0.000 title claims description 27
- 239000000463 material Substances 0.000 title claims description 13
- 239000011505 plaster Substances 0.000 title description 3
- 229920002725 thermoplastic elastomer Polymers 0.000 claims description 126
- 239000002480 mineral oil Substances 0.000 claims description 62
- 235000010446 mineral oil Nutrition 0.000 claims description 60
- 235000015112 vegetable and seed oil Nutrition 0.000 claims description 55
- 239000008158 vegetable oil Substances 0.000 claims description 55
- 229920005989 resin Polymers 0.000 claims description 53
- 239000011347 resin Substances 0.000 claims description 53
- 239000012188 paraffin wax Substances 0.000 claims description 39
- -1 polyethylene Polymers 0.000 claims description 27
- 229930195733 hydrocarbon Natural products 0.000 claims description 21
- 150000002430 hydrocarbons Chemical class 0.000 claims description 21
- 239000004793 Polystyrene Substances 0.000 claims description 19
- 125000004432 carbon atom Chemical group C* 0.000 claims description 19
- 229920002223 polystyrene Polymers 0.000 claims description 19
- 239000010440 gypsum Substances 0.000 claims description 14
- 229910052602 gypsum Inorganic materials 0.000 claims description 14
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 11
- 229920001400 block copolymer Polymers 0.000 claims description 11
- 239000004698 Polyethylene Substances 0.000 claims description 10
- 229920000573 polyethylene Polymers 0.000 claims description 10
- 238000000465 moulding Methods 0.000 claims description 8
- BXOUVIIITJXIKB-UHFFFAOYSA-N ethene;styrene Chemical group C=C.C=CC1=CC=CC=C1 BXOUVIIITJXIKB-UHFFFAOYSA-N 0.000 claims description 7
- 239000002245 particle Substances 0.000 claims description 7
- 239000000853 adhesive Substances 0.000 claims description 6
- 230000001070 adhesive effect Effects 0.000 claims description 6
- 150000004945 aromatic hydrocarbons Chemical class 0.000 claims description 5
- 239000011258 core-shell material Substances 0.000 claims description 5
- 239000008187 granular material Substances 0.000 claims description 5
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 claims description 5
- 239000004567 concrete Substances 0.000 claims description 4
- 239000003795 chemical substances by application Substances 0.000 claims description 2
- 239000010690 paraffinic oil Substances 0.000 claims 1
- 238000004898 kneading Methods 0.000 description 17
- 238000002156 mixing Methods 0.000 description 13
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 11
- 238000000034 method Methods 0.000 description 10
- 230000007704 transition Effects 0.000 description 10
- NOPFSRXAKWQILS-UHFFFAOYSA-N docosan-1-ol Chemical compound CCCCCCCCCCCCCCCCCCCCCCO NOPFSRXAKWQILS-UHFFFAOYSA-N 0.000 description 9
- 238000002844 melting Methods 0.000 description 9
- 230000008018 melting Effects 0.000 description 9
- RZJRJXONCZWCBN-UHFFFAOYSA-N octadecane Chemical compound CCCCCCCCCCCCCCCCCC RZJRJXONCZWCBN-UHFFFAOYSA-N 0.000 description 9
- 238000007711 solidification Methods 0.000 description 9
- 230000008023 solidification Effects 0.000 description 9
- DCAYPVUWAIABOU-UHFFFAOYSA-N hexadecane Chemical compound CCCCCCCCCCCCCCCC DCAYPVUWAIABOU-UHFFFAOYSA-N 0.000 description 8
- 239000008188 pellet Substances 0.000 description 8
- BGHCVCJVXZWKCC-UHFFFAOYSA-N tetradecane Chemical compound CCCCCCCCCCCCCC BGHCVCJVXZWKCC-UHFFFAOYSA-N 0.000 description 8
- 239000004743 Polypropylene Substances 0.000 description 7
- 150000001875 compounds Chemical class 0.000 description 7
- NDJKXXJCMXVBJW-UHFFFAOYSA-N heptadecane Chemical compound CCCCCCCCCCCCCCCCC NDJKXXJCMXVBJW-UHFFFAOYSA-N 0.000 description 7
- 238000012360 testing method Methods 0.000 description 7
- YCOZIPAWZNQLMR-UHFFFAOYSA-N heptane - octane Natural products CCCCCCCCCCCCCCC YCOZIPAWZNQLMR-UHFFFAOYSA-N 0.000 description 6
- 238000004519 manufacturing process Methods 0.000 description 6
- 229920005992 thermoplastic resin Polymers 0.000 description 6
- 239000004215 Carbon black (E152) Substances 0.000 description 5
- 230000000052 comparative effect Effects 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 238000005191 phase separation Methods 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- 229920002943 EPDM rubber Polymers 0.000 description 4
- 229920000181 Ethylene propylene rubber Polymers 0.000 description 4
- 229920002633 Kraton (polymer) Polymers 0.000 description 4
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 4
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 4
- 229910052799 carbon Inorganic materials 0.000 description 4
- 229960000735 docosanol Drugs 0.000 description 4
- CBFCDTFDPHXCNY-UHFFFAOYSA-N icosane Chemical compound CCCCCCCCCCCCCCCCCCCC CBFCDTFDPHXCNY-UHFFFAOYSA-N 0.000 description 4
- 229910052500 inorganic mineral Inorganic materials 0.000 description 4
- 239000011707 mineral Substances 0.000 description 4
- 238000007789 sealing Methods 0.000 description 4
- 239000005977 Ethylene Substances 0.000 description 3
- 230000000740 bleeding effect Effects 0.000 description 3
- 238000013329 compounding Methods 0.000 description 3
- 229920001577 copolymer Polymers 0.000 description 3
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 3
- 239000003822 epoxy resin Substances 0.000 description 3
- 238000011156 evaluation Methods 0.000 description 3
- 238000001125 extrusion Methods 0.000 description 3
- 230000005865 ionizing radiation Effects 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- 239000000178 monomer Substances 0.000 description 3
- 239000003921 oil Substances 0.000 description 3
- 235000019198 oils Nutrition 0.000 description 3
- 229920000647 polyepoxide Polymers 0.000 description 3
- 229920001155 polypropylene Polymers 0.000 description 3
- 229920002742 polystyrene-block-poly(ethylene/propylene) -block-polystyrene Polymers 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 239000011342 resin composition Substances 0.000 description 3
- 239000002023 wood Substances 0.000 description 3
- 229920000178 Acrylic resin Polymers 0.000 description 2
- 239000004925 Acrylic resin Substances 0.000 description 2
- 241000196324 Embryophyta Species 0.000 description 2
- JOYRKODLDBILNP-UHFFFAOYSA-N Ethyl urethane Chemical compound CCOC(N)=O JOYRKODLDBILNP-UHFFFAOYSA-N 0.000 description 2
- 238000003917 TEM image Methods 0.000 description 2
- 239000000654 additive Substances 0.000 description 2
- 238000004378 air conditioning Methods 0.000 description 2
- 125000003118 aryl group Chemical group 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000000748 compression moulding Methods 0.000 description 2
- 239000000470 constituent Substances 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 238000005520 cutting process Methods 0.000 description 2
- 230000003247 decreasing effect Effects 0.000 description 2
- 229920001971 elastomer Polymers 0.000 description 2
- 239000000806 elastomer Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000005038 ethylene vinyl acetate Substances 0.000 description 2
- 239000011094 fiberboard Substances 0.000 description 2
- 229920001903 high density polyethylene Polymers 0.000 description 2
- 239000004700 high-density polyethylene Substances 0.000 description 2
- BTFJIXJJCSYFAL-UHFFFAOYSA-N icosan-1-ol Chemical compound CCCCCCCCCCCCCCCCCCCCO BTFJIXJJCSYFAL-UHFFFAOYSA-N 0.000 description 2
- 238000001746 injection moulding Methods 0.000 description 2
- 239000000155 melt Substances 0.000 description 2
- LQERIDTXQFOHKA-UHFFFAOYSA-N nonadecane Chemical compound CCCCCCCCCCCCCCCCCCC LQERIDTXQFOHKA-UHFFFAOYSA-N 0.000 description 2
- 239000002667 nucleating agent Substances 0.000 description 2
- GLDOVTGHNKAZLK-UHFFFAOYSA-N octadecan-1-ol Chemical compound CCCCCCCCCCCCCCCCCCO GLDOVTGHNKAZLK-UHFFFAOYSA-N 0.000 description 2
- 239000005022 packaging material Substances 0.000 description 2
- 229920003023 plastic Polymers 0.000 description 2
- 229920001200 poly(ethylene-vinyl acetate) Polymers 0.000 description 2
- 229920005668 polycarbonate resin Polymers 0.000 description 2
- 239000004431 polycarbonate resin Substances 0.000 description 2
- 229920001225 polyester resin Polymers 0.000 description 2
- 239000004645 polyester resin Substances 0.000 description 2
- 229920005990 polystyrene resin Polymers 0.000 description 2
- 229920005996 polystyrene-poly(ethylene-butylene)-polystyrene Polymers 0.000 description 2
- 229920002743 polystyrene-poly(ethylene-ethylene/propylene) block-polystyrene Polymers 0.000 description 2
- 238000012545 processing Methods 0.000 description 2
- 238000000746 purification Methods 0.000 description 2
- 229920002050 silicone resin Polymers 0.000 description 2
- 239000010729 system oil Substances 0.000 description 2
- 229920002803 thermoplastic polyurethane Polymers 0.000 description 2
- 229920001187 thermosetting polymer Polymers 0.000 description 2
- IIYFAKIEWZDVMP-UHFFFAOYSA-N tridecane Chemical compound CCCCCCCCCCCCC IIYFAKIEWZDVMP-UHFFFAOYSA-N 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- ALSTYHKOOCGGFT-KTKRTIGZSA-N (9Z)-octadecen-1-ol Chemical compound CCCCCCCC\C=C/CCCCCCCCO ALSTYHKOOCGGFT-KTKRTIGZSA-N 0.000 description 1
- DNIAPMSPPWPWGF-GSVOUGTGSA-N (R)-(-)-Propylene glycol Chemical class C[C@@H](O)CO DNIAPMSPPWPWGF-GSVOUGTGSA-N 0.000 description 1
- 238000005160 1H NMR spectroscopy Methods 0.000 description 1
- 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 1
- LCZVSXRMYJUNFX-UHFFFAOYSA-N 2-[2-(2-hydroxypropoxy)propoxy]propan-1-ol Chemical compound CC(O)COC(C)COC(C)CO LCZVSXRMYJUNFX-UHFFFAOYSA-N 0.000 description 1
- TXBCBTDQIULDIA-UHFFFAOYSA-N 2-[[3-hydroxy-2,2-bis(hydroxymethyl)propoxy]methyl]-2-(hydroxymethyl)propane-1,3-diol Chemical compound OCC(CO)(CO)COCC(CO)(CO)CO TXBCBTDQIULDIA-UHFFFAOYSA-N 0.000 description 1
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical compound [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 description 1
- JLBJTVDPSNHSKJ-UHFFFAOYSA-N 4-Methylstyrene Chemical compound CC1=CC=C(C=C)C=C1 JLBJTVDPSNHSKJ-UHFFFAOYSA-N 0.000 description 1
- 235000017166 Bambusa arundinacea Nutrition 0.000 description 1
- 235000017491 Bambusa tulda Nutrition 0.000 description 1
- 244000025254 Cannabis sativa Species 0.000 description 1
- 229920008347 Cellulose acetate propionate Polymers 0.000 description 1
- 229920000089 Cyclic olefin copolymer Polymers 0.000 description 1
- 239000004593 Epoxy Substances 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
- 239000004594 Masterbatch (MB) Substances 0.000 description 1
- 239000004640 Melamine resin Substances 0.000 description 1
- 229920000877 Melamine resin Polymers 0.000 description 1
- WHNWPMSKXPGLAX-UHFFFAOYSA-N N-Vinyl-2-pyrrolidone Chemical compound C=CN1CCCC1=O WHNWPMSKXPGLAX-UHFFFAOYSA-N 0.000 description 1
- 244000082204 Phyllostachys viridis Species 0.000 description 1
- 235000015334 Phyllostachys viridis Nutrition 0.000 description 1
- 239000004952 Polyamide Substances 0.000 description 1
- 239000004721 Polyphenylene oxide Substances 0.000 description 1
- 229920001807 Urea-formaldehyde Polymers 0.000 description 1
- XTXRWKRVRITETP-UHFFFAOYSA-N Vinyl acetate Chemical compound CC(=O)OC=C XTXRWKRVRITETP-UHFFFAOYSA-N 0.000 description 1
- 229920002522 Wood fibre Polymers 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 230000004520 agglutination Effects 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 150000001336 alkenes Chemical group 0.000 description 1
- 229920000180 alkyd Polymers 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 230000003078 antioxidant effect Effects 0.000 description 1
- 239000002216 antistatic agent Substances 0.000 description 1
- 239000011425 bamboo Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000000071 blow moulding Methods 0.000 description 1
- QHIWVLPBUQWDMQ-UHFFFAOYSA-N butyl prop-2-enoate;methyl 2-methylprop-2-enoate;prop-2-enoic acid Chemical compound OC(=O)C=C.COC(=O)C(C)=C.CCCCOC(=O)C=C QHIWVLPBUQWDMQ-UHFFFAOYSA-N 0.000 description 1
- ZOMBKNNSYQHRCA-UHFFFAOYSA-J calcium sulfate hemihydrate Chemical compound O.[Ca+2].[Ca+2].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O ZOMBKNNSYQHRCA-UHFFFAOYSA-J 0.000 description 1
- 229920006026 co-polymeric resin Polymers 0.000 description 1
- 238000005345 coagulation Methods 0.000 description 1
- 230000015271 coagulation Effects 0.000 description 1
- 239000003086 colorant Substances 0.000 description 1
- 238000012790 confirmation Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 150000001993 dienes Chemical class 0.000 description 1
- 238000000113 differential scanning calorimetry Methods 0.000 description 1
- 239000003085 diluting agent Substances 0.000 description 1
- 239000002270 dispersing agent Substances 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
- SNRUBQQJIBEYMU-UHFFFAOYSA-N dodecane Chemical compound CCCCCCCCCCCC SNRUBQQJIBEYMU-UHFFFAOYSA-N 0.000 description 1
- 238000004043 dyeing Methods 0.000 description 1
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000003063 flame retardant Substances 0.000 description 1
- 235000013305 food Nutrition 0.000 description 1
- 238000009472 formulation Methods 0.000 description 1
- 125000000524 functional group Chemical group 0.000 description 1
- 239000011507 gypsum plaster Substances 0.000 description 1
- LNEPOXFFQSENCJ-UHFFFAOYSA-N haloperidol Chemical compound C1CC(O)(C=2C=CC(Cl)=CC=2)CCN1CCCC(=O)C1=CC=C(F)C=C1 LNEPOXFFQSENCJ-UHFFFAOYSA-N 0.000 description 1
- ACCCMOQWYVYDOT-UHFFFAOYSA-N hexane-1,1-diol Chemical compound CCCCCC(O)O ACCCMOQWYVYDOT-UHFFFAOYSA-N 0.000 description 1
- XXMIOPMDWAUFGU-UHFFFAOYSA-N hexane-1,6-diol Chemical compound OCCCCCCO XXMIOPMDWAUFGU-UHFFFAOYSA-N 0.000 description 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 238000010191 image analysis Methods 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 238000009413 insulation Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000000314 lubricant Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003607 modifier Substances 0.000 description 1
- 229940094933 n-dodecane Drugs 0.000 description 1
- GOQYKNQRPGWPLP-UHFFFAOYSA-N n-heptadecyl alcohol Natural products CCCCCCCCCCCCCCCCCO GOQYKNQRPGWPLP-UHFFFAOYSA-N 0.000 description 1
- SLCVBVWXLSEKPL-UHFFFAOYSA-N neopentyl glycol Chemical compound OCC(C)(C)CO SLCVBVWXLSEKPL-UHFFFAOYSA-N 0.000 description 1
- 229940038384 octadecane Drugs 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 229940055577 oleyl alcohol Drugs 0.000 description 1
- XMLQWXUVTXCDDL-UHFFFAOYSA-N oleyl alcohol Natural products CCCCCCC=CCCCCCCCCCCO XMLQWXUVTXCDDL-UHFFFAOYSA-N 0.000 description 1
- 150000001451 organic peroxides Chemical class 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 239000000123 paper Substances 0.000 description 1
- WXZMFSXDPGVJKK-UHFFFAOYSA-N pentaerythritol Chemical compound OCC(CO)(CO)CO WXZMFSXDPGVJKK-UHFFFAOYSA-N 0.000 description 1
- 239000003208 petroleum Substances 0.000 description 1
- 239000003209 petroleum derivative Substances 0.000 description 1
- 229920001568 phenolic resin Polymers 0.000 description 1
- 239000005011 phenolic resin Substances 0.000 description 1
- 239000010773 plant oil Substances 0.000 description 1
- 239000004033 plastic Substances 0.000 description 1
- 239000002985 plastic film Substances 0.000 description 1
- 229920003207 poly(ethylene-2,6-naphthalate) Polymers 0.000 description 1
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 1
- 229920002037 poly(vinyl butyral) polymer Polymers 0.000 description 1
- 229920002647 polyamide Polymers 0.000 description 1
- 150000004291 polyenes Chemical class 0.000 description 1
- 229920000570 polyether Polymers 0.000 description 1
- 239000011112 polyethylene naphthalate Substances 0.000 description 1
- 229920013716 polyethylene resin Polymers 0.000 description 1
- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 239000002952 polymeric resin Substances 0.000 description 1
- 239000004926 polymethyl methacrylate Substances 0.000 description 1
- 229920005672 polyolefin resin Polymers 0.000 description 1
- 229920001296 polysiloxane Polymers 0.000 description 1
- 229920006295 polythiol Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000012779 reinforcing material Substances 0.000 description 1
- 238000010057 rubber processing Methods 0.000 description 1
- 229910001927 ruthenium tetroxide Inorganic materials 0.000 description 1
- 229920006395 saturated elastomer Polymers 0.000 description 1
- 150000003384 small molecules Chemical class 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 230000006641 stabilisation Effects 0.000 description 1
- 238000011105 stabilization Methods 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 229920006132 styrene block copolymer Polymers 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 125000000383 tetramethylene group Chemical group [H]C([H])([*:1])C([H])([H])C([H])([H])C([H])([H])[*:2] 0.000 description 1
- 239000006097 ultraviolet radiation absorber Substances 0.000 description 1
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- 230000000007 visual effect Effects 0.000 description 1
- 239000004636 vulcanized rubber Substances 0.000 description 1
- 230000002087 whitening effect Effects 0.000 description 1
- 239000002025 wood fiber Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K5/00—Use of organic ingredients
- C08K5/01—Hydrocarbons
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L101/00—Compositions of unspecified macromolecular compounds
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L53/00—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
- C08L53/02—Compositions of block copolymers containing at least one sequence of a polymer obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers of vinyl-aromatic monomers and conjugated dienes
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L91/00—Compositions of oils, fats or waxes; Compositions of derivatives thereof
-
- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K5/00—Heat-transfer, heat-exchange or heat-storage materials, e.g. refrigerants; Materials for the production of heat or cold by chemical reactions other than by combustion
- C09K5/02—Materials undergoing a change of physical state when used
- C09K5/06—Materials undergoing a change of physical state when used the change of state being from liquid to solid or vice versa
-
- E—FIXED CONSTRUCTIONS
- E04—BUILDING
- E04B—GENERAL BUILDING CONSTRUCTIONS; WALLS, e.g. PARTITIONS; ROOFS; FLOORS; CEILINGS; INSULATION OR OTHER PROTECTION OF BUILDINGS
- E04B1/00—Constructions in general; Structures which are not restricted either to walls, e.g. partitions, or floors or ceilings or roofs
- E04B1/62—Insulation or other protection; Elements or use of specified material therefor
- E04B1/74—Heat, sound or noise insulation, absorption, or reflection; Other building methods affording favourable thermal or acoustical conditions, e.g. accumulating of heat within walls
- E04B1/76—Heat, sound or noise insulation, absorption, or reflection; Other building methods affording favourable thermal or acoustical conditions, e.g. accumulating of heat within walls specifically with respect to heat only
Description
本発明は、熱可塑性エラストマー組成物、成形体、建材、建材ボード、および塗り壁材に関する。 The present invention relates to thermoplastic elastomer compositions, molded bodies, building materials, building material boards, and plastered wall materials.
物質の相転移潜熱を蓄熱に利用する技術が知られている。その中でも、ｎ−パラフィンの相転移潜熱を利用する技術は、炭素数が１２から５０の範囲のｎ−パラフィンから適切な選択を行うことにより、広範な生活環境温度（−２０℃〜１００℃）に対応した相転移温度が利用可能であって、蓄熱密度が高く、相変化を繰り返しても特性が劣化しない、腐食性がない等の優れた特徴を有している。 A technique is known that utilizes the latent heat of the phase transition of a substance for heat storage. Among them, the technology utilizing the latent heat of the phase transition of n-paraffin has a wide range of living environment temperatures (-20 ° C to 100 ° C) by making an appropriate selection from n-paraffin having 12 to 50 carbon atoms. The phase transition temperature corresponding to the above is available, the heat storage density is high, the characteristics do not deteriorate even if the phase change is repeated, and there is no corrosiveness.
ｎ−パラフィンの蓄熱材料としての優れた特性を生かした蓄熱材として、熱可塑性エラストマーを担持材料とし、ｎ−パラフィンを溶融混練で固定化（ゲル化）した蓄熱材が提案されている。 As a heat storage material utilizing the excellent properties of n-paraffin as a heat storage material, a heat storage material in which a thermoplastic elastomer is used as a supporting material and n-paraffin is immobilized (gelled) by melt-kneading has been proposed.
近年、熱可塑性エラストマーの1種として、エチレン−エチレン／ブチレン−エチレンブロック共重合体（以下、「ＣＥＢＣ」と略すことがある）等の水添ジエン系共重合を使用する蓄熱材組成物が開発されている（例えば、特許文献１〜３参照）。 In recent years, as a type of thermoplastic elastomer, a heat storage material composition using a hydrogenated diene-based copolymer such as an ethylene-ethylene / butylene-ethylene block copolymer (hereinafter, may be abbreviated as "CEBC") has been developed. (See, for example, Patent Documents 1 to 3).
また、パラフィン系ワックスを蓄熱材料として使用し、スチレン−エチレン−エチレン／プロピレン−スチレン共重合体（以下、「ＳＥＥＰＳ」と略すことがある）を担持材料とする蓄熱材組成物も提案されている（例えば、特許文献４参照）。 Further, a heat storage material composition using a paraffin wax as a heat storage material and a styrene-ethylene-ethylene / propylene-styrene copolymer (hereinafter, sometimes abbreviated as "SEEPS") as a supporting material has also been proposed. (See, for example, Patent Document 4).
さらに、蓄熱材以外に加硫ゴム代替品として、パラフィン系化合物等の非芳香族系軟化剤と、スチレン−エチレン／プロピレン−スチレンブロック共重合体（以下、「ＳＥＰＳ」と略すことがある）、および／またはＣＥＢＣ等の熱可塑性エラストマーと、熱可塑性樹脂と、有機過酸化物とを含む熱可塑性エラストマー組成物も提案されている（例えば、特許文献５参照）。 Further, as a substitute for vulcanized rubber other than the heat storage material, a non-aromatic softener such as a paraffin compound, a styrene-ethylene / propylene-styrene block copolymer (hereinafter, may be abbreviated as "SEPS"), And / or a thermoplastic elastomer composition containing a thermoplastic elastomer such as CEBC, a thermoplastic resin, and an organic peroxide has also been proposed (see, for example, Patent Document 5).
特許文献１〜５で使用される熱可塑性エラストマーのＣＥＢＣ、ＳＥＥＰＳおよびＳＥＰＳは、従来使用されるスチレン−エチレン／ブチレン−スチレンブロック共重合体（ＳＥＢＳ）と比較して、パラフィン系化合物等の低分子量化合物の漏洩を防止しうる。しかしながら、上記の熱可塑性エラストマーを使用した場合でも、耐ブリード性は充分ではなかった。特に、相転移温度を挟んで温度を繰り返し上昇下降させる、所謂、ヒートサイクルの試験を行うと、熱可塑性エラストマー組成物の成形体からパラフィン系化合物等の低分子量化合物の滲み出しや相分離などの不具合を起こす場合がある。さらに、成形体を包装材料や容器に封入せずに使用する際、生活環境温度範囲で成形された形状を保持でき、安全性の観点から蓄熱材料の滲み出しがほとんどないことが要求される。 The thermoplastic elastomers CEBC, SEEPS and SEPS used in Patent Documents 1 to 5 have lower molecular weights such as paraffin compounds as compared with the conventionally used styrene-ethylene / butylene-styrene block copolymers (SEBS). It can prevent the leakage of compounds. However, even when the above thermoplastic elastomer was used, the bleed resistance was not sufficient. In particular, when a so-called heat cycle test is performed in which the temperature is repeatedly raised and lowered with the phase transition temperature in between, low molecular weight compounds such as paraffin compounds are exuded from the molded product of the thermoplastic elastomer composition and phase separation is observed. May cause problems. Further, when the molded product is used without being enclosed in a packaging material or a container, it is required that the molded product can maintain the molded shape within the living environment temperature range and that the heat storage material hardly exudes from the viewpoint of safety.
本発明は、上記に鑑みてなされたものであって、パラフィン系化合物等の鉱物系油の滲み出しや相分離がなく、包装材料等に封入することなく所望の形状に成形されて使用される際に、生活環境温度範囲で形状を保持可能な熱可塑性エラストマー組成物、成形体、建材、建材ボード、および塗り壁材を提供することにある。 The present invention has been made in view of the above, and is used after being molded into a desired shape without exudation or phase separation of mineral oils such as paraffinic compounds and without being sealed in a packaging material or the like. It is an object of the present invention to provide a thermoplastic elastomer composition, a molded product, a building material, a building material board, and a coated wall material capable of maintaining a shape in a living environment temperature range.
本発明者らは、上記課題を解決すべく、鋭意検討を進めた結果、ハードセグメントとしてポリスチレンブロックを分子中に１つのみ有する熱可塑性エラストマーが、パラフィン系化合物等を安定的に担持可能であること、また、ポリスチレンブロックを分子中に１つのみ有する熱可塑性エラストマーと、鉱物系油等と、樹脂成分とを配合することにより、生活環境温度範囲で成形された形状を保持でき、かつ鉱物系油等の耐ブリード性に極めて優れることを見出し、本発明を完成させるに至った。 As a result of diligent studies to solve the above problems, the present inventors can stably support a paraffin-based compound or the like with a thermoplastic elastomer having only one polystyrene block in the molecule as a hard segment. In addition, by blending a thermoplastic elastomer having only one polystyrene block in the molecule, mineral oil, etc., and a resin component, the shape formed in the living environment temperature range can be maintained and the shape is mineral-based. We have found that the bleed resistance of oil and the like is extremely excellent, and have completed the present invention.
すなわち、本発明の熱可塑性エラストマー組成物は、分子中にポリスチレンブロックを１つのみ有する熱可塑性エラストマー（Ａ）と、芳香族炭化水素、ナフテン系炭化水素およびパラフィン系炭化水素の混合物であって、ナフテン系炭化水素またはパラフィン系炭化水素の割合が最大である鉱物系油、またはパラフィン系炭化水素からなる植物系油（Ｂ）と、樹脂成分（Ｃ）と、を含むことを特徴とする。 That is, the thermoplastic elastomer composition of the present invention is a mixture of a thermoplastic elastomer (A) having only one polystyrene block in the molecule, an aromatic hydrocarbon, a naphthenic hydrocarbon, and a paraffinic hydrocarbon. It is characterized by containing a mineral oil having the largest proportion of naphthenic hydrocarbons or paraffinic hydrocarbons, or a vegetable oil (B) composed of paraffinic hydrocarbons, and a resin component (C).
また、本発明の成形体は、上記に記載の熱可塑性エラストマー組成物を成形してなることを特徴とする。 Further, the molded product of the present invention is characterized in that the thermoplastic elastomer composition described above is molded.
また、本発明の建材は、前記鉱物系油または植物系油（Ｂ）として、炭素数１４以上２０以下のｎ−パラフィンを５０質量％以上含む上記に記載の成形体を、石膏またはコンクリートに混合してなることを特徴とする。 Further, in the building material of the present invention, as the mineral oil or vegetable oil (B), the above-mentioned molded product containing 50% by mass or more of n-paraffin having 14 or more and 20 or less carbon atoms is mixed with gypsum or concrete. It is characterized by being made of.
また、本発明の建材ボードは、前記鉱物系油または植物系油（Ｂ）として、炭素数１４以上２０以下のｎ−パラフィンを５０質量％以上含む上記に記載の成形体および接着剤を用いてなることを特徴とする。 Further, the building material board of the present invention uses the above-mentioned molded body and adhesive containing 50% by mass or more of n-paraffin having 14 or more and 20 or less carbon atoms as the mineral oil or vegetable oil (B). It is characterized by becoming.
また、本発明の建材ボードは、前記鉱物系油または植物系油（Ｂ）として、炭素数１４以上２０以下のｎ−パラフィンを５０質量％以上含む上記に記載の成形体、小片および接着剤を用いてなることを特徴とする。 Further, the building material board of the present invention contains the above-mentioned molded body, small pieces and adhesive containing 50% by mass or more of n-paraffin having 14 or more and 20 or less carbon atoms as the mineral oil or vegetable oil (B). It is characterized by being used.
また、本発明の塗り壁材は、前記鉱物系油または植物系油（Ｂ）として、炭素数１４以上２０以下のｎ−パラフィンを５０質量％以上含む上記に記載の成形体を、石膏に混合してなることを特徴とする。 Further, in the plaster wall material of the present invention, as the mineral oil or plant oil (B), the above-mentioned molded product containing 50% by mass or more of n-paraffin having 14 or more and 20 or less carbon atoms is mixed with gypsum. It is characterized by being made of.
本発明によれば、鉱物系油の低分子量成分の滲み出しがなく、各構成成分が高い相溶性を有するとともに、生活環境温度範囲で形状を保持可能な熱可塑性エラストマー組成物、成形体、建材、建材ボード、および塗り壁材を提供することが可能となる。 According to the present invention, there is no exudation of low molecular weight components of mineral oil, each component has high compatibility, and a thermoplastic elastomer composition, a molded product, and a building material capable of maintaining a shape within a living environment temperature range. , Building material boards, and coated wall materials can be provided.
本発明に係る熱可塑性エラストマー組成物、成形体、建材、建材ボード、および塗り壁材の好適な実施形態について、更に詳細に説明するが、以下に記載する構成要件の説明は、本発明の実施態様の一例であり、本発明はこれらの内容に限定されるものではなく、その要旨の範囲内で種々変形して実施することができる。 Preferable embodiments of the thermoplastic elastomer composition, molded article, building material, building material board, and coated wall material according to the present invention will be described in more detail, but the description of the constituent requirements described below is the embodiment of the present invention. It is an example of an embodiment, and the present invention is not limited to these contents, and can be carried out with various modifications within the scope of the gist thereof.
本発明に係る熱可塑性エラストマー組成物は、ポリスチレンブロックを分子中に１つのみ有する熱可塑性エラストマー（Ａ）と、鉱物系油または植物系油（Ｂ）と、樹脂成分（Ｃ）と、を含むことを特徴とする。以下、構成成分について順次説明する。 The thermoplastic elastomer composition according to the present invention contains a thermoplastic elastomer (A) having only one polystyrene block in the molecule, a mineral oil or a vegetable oil (B), and a resin component (C). It is characterized by that. Hereinafter, the constituent components will be described in order.
＜熱可塑性エラストマー（Ａ）＞
本発明にかかる熱可塑性エラストマー（Ａ）は、分子中にポリスチレンブロックを１つのみ有する熱可塑性エラストマーである。本発明の熱可塑性エラストマー（Ａ）は、スチレンを繰り返し単位とする結晶構造であるハードセグメントブロックと、水素添加処理後も共役ジエン化合物に由来する分岐の存在により非晶構造であるソフトセグメントブロックを有するものであって、ハードセグメントブロックとしてポリスチレンブロックを１つのみ有している。１Ｈ−ＮＭＲで構造決定を行えば、オレフィン領域に検出される水素原子は極めて微量（数％以下）である。なお、本発明の熱可塑性エラストマー（Ａ）は、ポリスチレンブロックが１つであれば、ポリスチレンブロック以外のハードセグメントブロックを有していてもよい。<Thermoplastic elastomer (A)>
The thermoplastic elastomer (A) according to the present invention is a thermoplastic elastomer having only one polystyrene block in the molecule. The thermoplastic elastomer (A) of the present invention comprises a hard segment block having a crystal structure having styrene as a repeating unit and a soft segment block having an amorphous structure due to the presence of branches derived from a conjugated diene compound even after hydrogenation treatment. It has only one polystyrene block as a hard segment block. 1 When the structure is determined by 1 H-NMR, the amount of hydrogen atoms detected in the olefin region is extremely small (several% or less). The thermoplastic elastomer (A) of the present invention may have a hard segment block other than the polystyrene block as long as it has one polystyrene block.
熱可塑性エラストマー（Ａ）は、ポリスチレンブロックが疑似架橋して球形コロイド粒子を形成する。形成された球形コロイド粒子の凝集によってソフトセグメントの間に隙間が生じ、この隙間に後述する鉱物系油または植物系油（Ｂ）は微分散されると推定される。熱可塑性エラストマー（Ａ）は、分子内にポリスチレンブロックを１つしか有さず、鉱物系油または植物系油（Ｂ）が分散しうる空間が大きいため、分子内にポリスチレンブロックを２つ有する熱可塑性エラストマーに比べて、鉱物系油または植物系油（Ｂ）を安定して担持でき、鉱物系油または植物系油（Ｂ）のブリードを防止することができる。また、ハードセグメントとしてポリスチレンブロックを有していない、エチレン−エチレン／ブチレン−エチレンブロック共重合体（ＣＥＢＣ）は、結晶性のポリエチレンブロックの疑似架橋を形成すると推測されるが、ポリスチレンブロックの疑似架橋より弱く、蓄熱材料の担持性能に劣るものと推定される。 In the thermoplastic elastomer (A), polystyrene blocks are pseudo-crosslinked to form spherical colloidal particles. It is presumed that the agglutination of the formed spherical colloidal particles creates a gap between the soft segments, and the mineral oil or vegetable oil (B) described later is finely dispersed in the gap. The thermoplastic elastomer (A) has only one polystyrene block in the molecule, and since there is a large space in which the mineral oil or the vegetable oil (B) can be dispersed, the heat having two polystyrene blocks in the molecule. Compared with the plastic elastomer, the mineral oil or the vegetable oil (B) can be stably supported, and the bleeding of the mineral oil or the vegetable oil (B) can be prevented. Further, it is presumed that ethylene-ethylene / butylene-ethylene block copolymer (CEBC), which does not have a polystyrene block as a hard segment, forms pseudo-crosslinks of crystalline polyethylene blocks, but pseudo-crosslinks of polystyrene blocks. It is presumed to be weaker and inferior in the carrying performance of the heat storage material.
ポリスチレンブロックを分子中に１つのみ有する熱可塑性エラストマー（Ａ）としては、２つのブロックを有するジブロック体、例えば、ハードセグメントブロックとしてポリスチレンブロックを１つと、ソフトセグメントブロックを１つ有するものが好ましい。熱可塑性エラストマー（Ａ）のジブロック体として、スチレン−エチレン／プロピレンブロック共重合体（以下、「ＳＥＰ」と略すことがある）、スチレン−エチレン／ブチレンブロック共重合体（以下、「ＳＥＢ」と略すことがある）、スチレン−イソブチレン共重合体（以下、「ＳＩＢ」と略すことがある）等が例示される。スチレン−エチレン／プロピレンブロック共重合体としては、例えば、クレイトンポリマージャパン（株）からクレイトン（登録商標）Ｇ（ＳＥＰタイプ）、「１７０１ＥＵ」、「１７０２ＨＵ」の商品名で販売されるものが例示される。 As the thermoplastic elastomer (A) having only one polystyrene block in the molecule, a diblock body having two blocks, for example, one having one polystyrene block and one soft segment block as a hard segment block is preferable. .. As the diblock body of the thermoplastic elastomer (A), a styrene-ethylene / propylene block copolymer (hereinafter, may be abbreviated as "SEP") and a styrene-ethylene / butylene block copolymer (hereinafter, "SEB") (May be abbreviated), styrene-isobutylene copolymer (hereinafter, may be abbreviated as “SIB”) and the like are exemplified. Examples of the styrene-ethylene / propylene block copolymer include those sold by Clayton Polymer Japan Co., Ltd. under the trade names of Clayton (registered trademark) G (SEP type), "1701EU", and "1702HU". To.
また、本発明で使用する熱可塑性エラストマー（Ａ）は、ポリエチレンブロックを含まないものが好ましい。鉱物系油または植物系油（Ｂ）としてｎ−パラフィンを使用する場合、分子内にポリエチレンブロックを有すると、このポリエチレンブロックにｎ−パラフィンが吸着することにより、蓄熱材として使用する際に蓄熱量が低下するためである。高い蓄熱量を有し、ブリードアウトを抑制する観点から、熱可塑性エラストマー（Ａ）は、分子中にポリスチレンブロックを１つのみ有し、ポリエチレンブロックを有しないＳＥＰを好適に使用することができる。 Further, the thermoplastic elastomer (A) used in the present invention preferably does not contain a polyethylene block. When n-paraffin is used as the mineral oil or vegetable oil (B), if a polyethylene block is provided in the molecule, the n-paraffin is adsorbed on the polyethylene block, so that the amount of heat stored when used as a heat storage material. This is because From the viewpoint of having a high heat storage amount and suppressing bleed-out, the thermoplastic elastomer (A) can preferably use SEP having only one polystyrene block in the molecule and not having a polyethylene block.
熱可塑性エラストマー（Ａ）は、示差走査式熱量測定法（ＤＳＣ法）により測定した場合に、ハードセグメント由来の融解ピークを有することが好ましく、８０〜１２０℃の範囲に融解ピークを有することが更に好ましい。 The thermoplastic elastomer (A) preferably has a melting peak derived from a hard segment when measured by a differential scanning calorimetry (DSC method), and further preferably has a melting peak in the range of 80 to 120 ° C. preferable.
熱可塑性エラストマー（Ａ）は、１種単独で用いることもできるが、２種以上を混合して用いることもできる。２種以上を混合して使用する場合には、少なくともスチレン−エチレン／プロピレンブロック共重合体を含むことが好ましい。 The thermoplastic elastomer (A) can be used alone or in combination of two or more. When two or more kinds are mixed and used, it is preferable to contain at least a styrene-ethylene / propylene block copolymer.
＜鉱物系油または植物系油（Ｂ）＞
本発明にかかる鉱物系油または植物系油（Ｂ）は、芳香族炭化水素、ナフテン系炭化水素およびパラフィン系炭化水素の混合物であって、ナフテン系炭化水素またはパラフィン系炭化水素の割合が最大である鉱物系油、またはパラフィン系炭化水素からなる植物系油（Ｂ）（以下、「鉱物系油または植物系油」と略す）である。鉱物系油は、パラフィン系炭化水素が鉱物系油中５０質量％以上のものをパラフィン系、ナフテン系炭化水素が３０〜４５質量％のものをナフテン系、芳香族炭化水素が３０質量％以上のものを芳香族系として区分されているが、本発明の鉱物系油は、鉱物系油中の成分のうち、ナフテン系炭化水素またはパラフィン系炭化水素の割合が最も大きいパラフィン系またはナフテン系の鉱物系油であり、芳香族炭化水素の割合が５質量％以下のものが好ましい。<Mineral oil or vegetable oil (B)>
The mineral oil or vegetable oil (B) according to the present invention is a mixture of aromatic hydrocarbons, naphthenic hydrocarbons and paraffinic hydrocarbons, and the ratio of naphthenic hydrocarbons or paraffinic hydrocarbons is maximum. A certain mineral oil or a vegetable oil (B) composed of a paraffinic hydrocarbon (hereinafter, abbreviated as "mineral oil or vegetable oil"). As for mineral oils, paraffin-based hydrocarbons having a paraffin-based hydrocarbon content of 50% by mass or more are paraffin-based, naphthen-based hydrocarbons having a content of 30 to 45% by mass are naphthen-based, and aromatic hydrocarbons having a content of 30% by mass or more. Although those are classified as aromatic, the mineral oil of the present invention is a paraffin-based or naphthen-based mineral having the largest proportion of naphthenic hydrocarbons or paraffinic hydrocarbons among the components in the mineral oil. It is a system oil, preferably one having an aromatic hydrocarbon content of 5% by mass or less.
本発明の熱可塑性エラストマー組成物を蓄熱材として使用する場合、鉱物系油または植物系油（Ｂ）は、パラフィン系炭化水素、好ましくは、相転移温度が−２０℃〜１００℃である、炭素数が１２以上５０以下のｎ−パラフィンが使用される。これらのｎ−パラフィンは、通常、石油留分から精留によって得られる。精製技術の制約から、それぞれの炭素数のｎ−パラフィンには、数質量％の隣接した炭素数のｎ−パラフィンを含有することがある。なお、蓄熱材に使用するｎ−パラフィンは、合成したものを使用してもよいが、石油留分由来のものを用いる方が、簡便かつ安価である。以下、本明細書では、精留によって得られた数質量％程度の不純物を含むｎ−パラフィン、または合成により得られた純度が高いｎ−パラフィンを、特に区別することなく、特定の炭素数を有するｎ−パラフィンとして記載する。 When the thermoplastic elastomer composition of the present invention is used as a heat storage material, the mineral oil or vegetable oil (B) is a paraffinic hydrocarbon, preferably carbon having a phase transition temperature of −20 ° C. to 100 ° C. N-paraffin having a number of 12 or more and 50 or less is used. These n-paraffins are usually obtained by rectification from petroleum distillates. Due to the limitation of purification technology, each n-paraffin having a carbon number may contain n-paraffin having an adjacent carbon number of several mass%. The n-paraffin used as the heat storage material may be a synthetic one, but it is simpler and cheaper to use one derived from petroleum fraction. Hereinafter, in the present specification, n-paraffin containing impurities of about several mass% obtained by rectification or n-paraffin having high purity obtained by synthesis is referred to as a specific carbon number without particular distinction. Described as having n-paraffin.
蓄熱材用の鉱物系油または植物系油（Ｂ）として特に有用なｎ−パラフィンは、相転移温度が、保冷〜住居環境温度範囲の−１０℃〜３５℃の範囲にある、炭素数が１２以上２０以下のｎ−パラフィンであり、例えば、ｎ−ドデカン、ｎ−トリデカン、ｎ−テトラデカン、ｎ−ペンタデカン、ｎ−ヘキサデカン、ｎ−ヘプタデカン、ｎ−オクタデカン、ｎ−ノナデカンおよびｎ−エイコサンの割合が５０質量％以上であることが好ましい。潜熱蓄熱材料として特に好ましいのは、相転移潜熱量の大きい、炭素数が偶数のｎ−テトラデカン、ｎ−ヘキサデカン、ｎ−オクタデカン、ｎ−エイコサンを主として含むものである。 N-paraffin, which is particularly useful as a mineral oil or vegetable oil (B) for a heat storage material, has a phase transition temperature in the range of -10 ° C to 35 ° C in the cold insulation to living environment temperature range, and has 12 carbon atoms. It is n-paraffin of 20 or more, and for example, the proportions of n-dodecane, n-tridecane, n-tetradecane, n-pentadecane, n-hexadecane, n-heptadecane, n-octadecane, n-nonadecane and n-icosane are It is preferably 50% by mass or more. Particularly preferable as the latent heat storage material, it mainly contains n-tetradecane, n-hexadecane, n-octadecane, and n-icosane having a large phase transition latent heat and an even number of carbon atoms.
蓄熱材用の鉱物系油または植物系油（Ｂ）は、炭素数が１４以上２０以下のｎ−パラフィンの割合が５０質量％以上であるものがより好ましく、炭素数が１４以上２０以下のｎ−パラフィンからなり、かつ、この範囲にあるいずれかのｎ−パラフィン、特にｎ−テトラデカン、ｎ−ヘキサデカン、ｎ−オクタデカン、またはｎ−エイコサンを５０質量％以上含むものが特に好ましい。 The mineral oil or vegetable oil (B) for the heat storage material is more preferably n-paraffin having 14 or more and 20 or less carbon atoms in an amount of 50% by mass or more, and n having 14 or more and 20 or less carbon atoms. It is particularly preferred that it consists of -paraffin and contains 50% by mass or more of any n-paraffin in this range, particularly n-tetradecane, n-hexadecane, n-octadecane, or n-icosane.
蓄熱材用の鉱物系油（Ｂ）としては、炭素数が１４以上２０以下のｎ−パラフィンからなり、かつ、この範囲にあるいずれかのｎ−パラフィン、特にｎ−テトラデカン、ｎ−ヘキサデカン、ｎ−オクタデカン、またはｎ−エイコサンを９５質量％以上含むものがさらに好ましい。 The mineral oil (B) for the heat storage material is composed of n-paraffin having 14 or more and 20 or less carbon atoms, and any n-paraffin in this range, particularly n-tetradecane, n-hexadecane, n. More preferably, it contains 95% by mass or more of −octadecane or n−icosane.
＜樹脂成分（Ｃ）＞
本発明にかかる樹脂成分（Ｃ）は、熱可塑性樹脂、電離放射線硬化型樹脂、および熱硬化性樹脂から選択される。
熱可塑性樹脂としては、アクリル系樹脂、ポリエステル系樹脂、ポリオレフィン系樹脂、ビニル系樹脂、ポリカーボネート系樹脂、およびポリスチレン系樹脂が例示され、中でも、ポリメタクリル酸メチル樹脂、ポリエチレンテレフタレート樹脂、ポリエチレンナフタレート樹脂、ポリプロピレン樹脂、ポリエチレン樹脂、ポリ塩化ビニル樹脂、シクロオレフィンポリマー樹脂、セルロースアセテートプロピオネート樹脂、ポリビニルブチラール樹脂、ポリカーボネート樹脂、ＥＰＤＭ（エチレン−プロピレン−ジエンゴム）、変性エチレン−プロピレンゴム（変性ＥＰＲ）、エチレン・酢酸ビニル共重合樹脂およびポリスチレン樹脂を用いることがより好ましい。これらの樹脂は、１種単独または２種以上を組み合わせて用いることができる。<Resin component (C)>
The resin component (C) according to the present invention is selected from a thermoplastic resin, an ionizing radiation curable resin, and a thermosetting resin.
Examples of the thermoplastic resin include acrylic resin, polyester resin, polyolefin resin, vinyl resin, polycarbonate resin, and polystyrene resin. Among them, polymethyl methacrylate resin, polyethylene terephthalate resin, and polyethylene naphthalate resin. , Polypropylene resin, polyethylene resin, polyvinyl chloride resin, cycloolefin polymer resin, cellulose acetate propionate resin, polyvinyl butyral resin, polycarbonate resin, EPDM (ethylene-propylene-diene rubber), modified ethylene-propylene rubber (modified EPR), It is more preferable to use an ethylene / vinyl acetate copolymer resin and a polystyrene resin. These resins can be used alone or in combination of two or more.
電離放射線硬化型樹脂としては、アクリル系やウレタン系、アクリルウレタン系やエポキシ系、シリコーン系樹脂等が挙げられる。これらの中でも、アクリレート系の官能基を有するもの、例えば比較的低分子量のポリエステル樹脂、ポリエーテル樹脂、アクリル樹脂、エポキシ樹脂、ウレタン樹脂、アルキッド樹脂、スピロアセタール樹脂、ポリブタジェン樹脂、ポリチオールポリエン樹脂、多価アルコール等の多官能化合物の（メタ）アルリレート等のオリゴマー又はプレポリマー及び反応性希釈剤としてエチル（メタ）アクリレート、エチルヘキシル（メタ）アクリレート、スチレン、メチルスチレン、Ｎ−ビニルピロリドン等の単官能モノマー並びに多官能モノマー、例えば、ポリメチロールプロパントリ（メタ）アクリレート、ヘキサンジオール（メタ）アクリレート、トリプロピレングリコールジ（メタ）アクリレート、ジエチレングリコールジ（メタ）アクリレート、ペンタエリスリトールトリ（メタ）アクリレート、ジペンタエリスリトールヘキサ（メタ）アクリレート、１，６−ヘキサンジオールジ（メタ）アクリレート、ネオペンチルグリコールジ（メタ）アクリレート等を比較的多量に含有するものが好ましい。また、電離放射線硬化型樹脂と熱可塑性樹脂とを溶剤により混合したものも使用することができる。 Examples of the ionizing radiation curable resin include acrylic-based and urethane-based resins, acrylic urethane-based and epoxy-based resins, and silicone-based resins. Among these, those having an acrylate-based functional group, for example, polyester resin having a relatively low molecular weight, polyether resin, acrylic resin, epoxy resin, urethane resin, alkyd resin, spiroacetal resin, polybutagen resin, polythiol polyene resin, many Monofunctional monomers such as (meth) alrilate of polyfunctional compounds such as valent alcohols, or monofunctional monomers such as ethyl (meth) acrylate, ethylhexyl (meth) acrylate, styrene, methylstyrene, and N-vinylpyrrolidone as reactive diluents. Also, polyfunctional monomers such as polymethylol propantri (meth) acrylate, hexanediol (meth) acrylate, tripropylene glycol di (meth) acrylate, diethylene glycol di (meth) acrylate, pentaerythritol tri (meth) acrylate, dipentaerythritol. Those containing a relatively large amount of hexa (meth) acrylate, 1,6-hexanediol di (meth) acrylate, neopentyl glycol di (meth) acrylate and the like are preferable. Further, a mixture of an ionizing radiation curable resin and a thermoplastic resin with a solvent can also be used.
熱硬化性樹脂としては、フェノール系樹脂、エポキシ系樹脂、シリコーン系樹脂、メラミン樹脂、ウレタン系樹脂、尿素樹脂等が挙げられる。これらの中でも、エポキシ系樹脂、シリコーン系樹脂が好ましい。 Examples of the thermosetting resin include phenolic resin, epoxy resin, silicone resin, melamine resin, urethane resin, urea resin and the like. Among these, epoxy resins and silicone resins are preferable.
本発明にかかる樹脂成分（Ｃ）としては、熱可塑性エラストマー組成物をフィルム状成型体、またはペレット等の粒状成形体に成形する際の成形性の観点から、熱可塑性樹脂を使用することが好ましい。 As the resin component (C) according to the present invention, it is preferable to use a thermoplastic resin from the viewpoint of moldability when molding the thermoplastic elastomer composition into a film-shaped molded product or a granular molded product such as pellets. ..
また、本発明にかかる熱可塑性エラストマー組成物は、炭素数１６以上２４以下の高級アルコール（Ｄ）を配合することもできる。熱可塑性エラストマー組成物を蓄熱材として使用する場合、熱可塑性エラストマー組成物に高級アルコール（Ｄ）を配合すると、鉱物系油または植物系油（Ｂ）が液体から固体に相変化する際、高級アルコールが核剤として機能し、熱可塑性エラストマー組成物の過冷却を防止することができる。 Further, the thermoplastic elastomer composition according to the present invention may also contain a higher alcohol (D) having 16 or more and 24 or less carbon atoms. When the thermoplastic elastomer composition is used as a heat storage material, when the higher alcohol (D) is added to the thermoplastic elastomer composition, the higher alcohol when the mineral oil or the vegetable oil (B) undergoes a phase change from a liquid to a solid. Acts as a nucleating agent and can prevent overcooling of the thermoplastic elastomer composition.
高級アルコール（Ｄ）としては、炭素数１６以上２４以下の直鎖状、または分岐鎖状の飽和、または不飽和の脂肪族アルコールが好ましく、例えば、ステアリルアルコール、ノナデシルアルコール、アラキジルアルコール、ヘンエイコサノール、ベヘニルアルコール、オレイルアルコール等を挙げることができる。中でも、ベヘニルアルコールが好ましい。 As the higher alcohol (D), a linear or branched saturated or unsaturated aliphatic alcohol having 16 to 24 carbon atoms is preferable, and for example, stearyl alcohol, nonadecil alcohol, arachidyl alcohol, and hen. Eikosanol, behenyl alcohol, oleyl alcohol and the like can be mentioned. Of these, behenyl alcohol is preferable.
高級アルコール（Ｄ）を配合する場合、鉱物系油または植物系油（Ｂ）１００質量部に対して１質量部以上５質量部以下の割合で配合することが好ましい。 When the higher alcohol (D) is blended, it is preferable to blend it in a ratio of 1 part by mass or more and 5 parts by mass or less with respect to 100 parts by mass of the mineral oil or the vegetable oil (B).
さらに、本発明の熱可塑性エラストマー組成物には、上記の原料成分以外にも、従来公知の添加剤を加えてもよい。添加剤としては、例えば、強化材、核剤、着色剤、酸化防止剤、帯電防止剤、滑剤、紫外線吸収剤、相溶化剤、難燃剤、防曇剤および安定剤等が挙げられる。 Further, conventionally known additives may be added to the thermoplastic elastomer composition of the present invention in addition to the above-mentioned raw material components. Examples of the additive include a reinforcing material, a nucleating agent, a coloring agent, an antioxidant, an antistatic agent, a lubricant, an ultraviolet absorber, a compatibilizer, a flame retardant, an antifogging agent and a stabilizer.
＜熱可塑性エラストマー組成物＞
本発明にかかる蓄熱樹脂組成物は、熱可塑性エラストマー（Ａ）を５質量％以上５０質量％以下、鉱物系油または植物系油（Ｂ）を３０質量％以上８０質量％以下、樹脂成分（Ｃ）を１０質量％以上６０質量％以下の割合で含むことが好ましい。熱可塑性エラストマー（Ａ）の割合が５質量％未満、または鉱物系油または植物系油（Ｂ）が８０質量％より大きい場合、鉱物系油または植物系油（Ｂ）が蓄熱樹脂組成物から漏れ出すおそれがある。また、熱可塑性エラストマー（Ａ）の割合が５０質量％より大きい、または鉱物系油または植物系油（Ｂ）が３０質量％未満の場合、成型性が悪くなるとともに、蓄熱材として使用する場合に十分な蓄熱量を確保できない場合がある。樹脂成分（Ｃ）の配合割合が１０質量％未満の場合、本発明の熱可塑性エラストマー組成物の成形体が生活環境温度範囲で形状を保持できないおそれがあり、樹脂成分（Ｃ）の配合割合が６０質量％より大きい場合、鉱物系油または植物系油（Ｂ）が熱可塑性エラストマー組成物から漏れ出したり、十分な蓄熱量を確保できない場合がある。熱可塑性エラストマー（Ａ）を１０質量％以上４０質量％以下、鉱物系油または植物系油（Ｂ）を４０質量％以上７０質量％以下、樹脂成分（Ｃ）を１５質量％以上５０質量％以下の割合で含むことがより好ましい。<Thermoplastic elastomer composition>
The heat storage resin composition according to the present invention contains 5% by mass or more and 50% by mass or less of the thermoplastic elastomer (A), 30% by mass or more and 80% by mass or less of the mineral oil or vegetable oil (B), and the resin component (C). ) Is preferably contained in a proportion of 10% by mass or more and 60% by mass or less. If the proportion of the thermoplastic elastomer (A) is less than 5% by mass, or the mineral oil or vegetable oil (B) is greater than 80% by mass, the mineral oil or vegetable oil (B) leaks from the heat storage resin composition. There is a risk of issuing it. Further, when the proportion of the thermoplastic elastomer (A) is larger than 50% by mass, or when the mineral oil or vegetable oil (B) is less than 30% by mass, the moldability deteriorates and when it is used as a heat storage material. It may not be possible to secure a sufficient amount of heat storage. If the blending ratio of the resin component (C) is less than 10% by mass, the molded product of the thermoplastic elastomer composition of the present invention may not retain its shape within the living environment temperature range, and the blending ratio of the resin component (C) is high. If it is larger than 60% by mass, the mineral oil or the vegetable oil (B) may leak from the thermoplastic elastomer composition, or a sufficient amount of heat storage may not be secured. Thermoplastic elastomer (A) is 10% by mass or more and 40% by mass or less, mineral oil or vegetable oil (B) is 40% by mass or more and 70% by mass or less, and resin component (C) is 15% by mass or more and 50% by mass or less. It is more preferable to include in the ratio of.
熱可塑性エラストマー組成物の成形体は、熱可塑性エラストマー（Ａ）および鉱物系油または植物系油（Ｂ）のリッチ相である島相と、樹脂成分（Ｃ）のリッチ相である海相とを有する海島構造をなす。図１は、実施例１０の熱可塑性エラストマー組成物の成形体断面の顕微鏡写真である（倍率５０００倍）。図１に示すように、本発明の熱可塑性エラストマー組成物の成形体は、白く見える樹脂成分（Ｃ）のリッチ相である海相（連続相）と、黒く見える熱可塑性エラストマー（Ａ）および鉱物系油または植物系油（Ｂ）のリッチ相である島相（分散相）をなしている。 The molded product of the thermoplastic elastomer composition comprises an island phase which is a rich phase of the thermoplastic elastomer (A) and a mineral oil or a vegetable oil (B) and a sea phase which is a rich phase of the resin component (C). It has a sea-island structure. FIG. 1 is a photomicrograph of a cross section of a molded product of the thermoplastic elastomer composition of Example 10 (magnification: 5000 times). As shown in FIG. 1, the molded product of the thermoplastic elastomer composition of the present invention has a sea phase (continuous phase) which is a rich phase of the resin component (C) that looks white, and a thermoplastic elastomer (A) and a mineral that look black. It forms an island phase (dispersed phase), which is a rich phase of a system oil or a vegetable oil (B).
図２は、図１の熱可塑性エラストマー組成物の成形体の断面（島相）の顕微鏡写真である（倍率１０００００倍）。図２に示すように、分散相である島相は、鉱物系油または植物系油（Ｂ）をコア、熱可塑性エラストマー（Ａ）をシェルとするコアシェル構造をなしている。このコアシェル構造により鉱物系油または植物系油（Ｂ）の耐ブリード性が著しく向上する。コアシェル構造の平均粒径は、１０〜５００ｎｍであることが好ましく、４０〜２００ｎｍがさらに好ましい。 FIG. 2 is a photomicrograph of a cross section (island phase) of the molded product of the thermoplastic elastomer composition of FIG. 1 (magnification: 100,000 times). As shown in FIG. 2, the island phase, which is a dispersed phase, has a core-shell structure in which a mineral oil or a vegetable oil (B) is used as a core and a thermoplastic elastomer (A) is used as a shell. This core-shell structure significantly improves the bleed resistance of the mineral oil or the vegetable oil (B). The average particle size of the core-shell structure is preferably 10 to 500 nm, more preferably 40 to 200 nm.
熱可塑性エラストマー組成物を蓄熱材として使用する場合、成形体の断面における海島構造の島相の面積が大きくなると、凝固熱量が高くなり好ましい。島相の割合は、熱可塑性エラストマー（Ａ）、鉱物系油または植物系油（Ｂ）および樹脂成分（Ｃ）の配合割合によって調整することができるが、樹脂成分（Ｃ）の配合割合が３５質量％を超えると、島相の割合が急激に低下する。これは、海相である樹脂成分（Ｃ）中に鉱物系油または植物系油（Ｂ）が拡散するためである。成形体の断面における海島構造の島相の面積は、６０％以上であることが好ましい。 When the thermoplastic elastomer composition is used as the heat storage material, it is preferable that the area of the island phase of the sea-island structure in the cross section of the molded product is large because the amount of heat of solidification is large. The ratio of the island phase can be adjusted by the blending ratio of the thermoplastic elastomer (A), the mineral oil or the vegetable oil (B) and the resin component (C), and the blending ratio of the resin component (C) is 35. If it exceeds% by mass, the proportion of island fauna drops sharply. This is because the mineral oil or the vegetable oil (B) diffuses into the resin component (C) which is the sea phase. The area of the island phase of the sea-island structure in the cross section of the molded body is preferably 60% or more.
＜熱可塑性エラストマー組成物の製造方法＞
次に、本発明の熱可塑性エラストマー組成物の製造方法の一例について説明する。
本発明にかかる熱可塑性エラストマー組成物は、所定量の熱可塑性エラストマー（Ａ）、鉱物系油または植物系油（Ｂ）、樹脂成分（Ｃ）、および配合する場合には高級アルコール（Ｄ）を機械的手段により強制的に混練、好ましくは、溶融混練して得ることができる（混練工程）。<Manufacturing method of thermoplastic elastomer composition>
Next, an example of the method for producing the thermoplastic elastomer composition of the present invention will be described.
The thermoplastic elastomer composition according to the present invention contains a predetermined amount of the thermoplastic elastomer (A), a mineral oil or a vegetable oil (B), a resin component (C), and a higher alcohol (D) when blended. It can be obtained by forcibly kneading by mechanical means, preferably melt-kneading (kneading step).
溶融混練は少なくとも熱可塑性エラストマー（Ａ）、鉱物系油または植物系油（Ｂ）、樹脂成分（Ｃ）が溶融する温度以上で行うことが好ましい。混合は機械的手段による混合である限り、各種の混合手段がいずれも採用され、代表的な手段として、撹拌、混合、混練であり、当該機能を有する機器としては、撹拌機、混合器、混練機、そして、ゴム加工や熱可塑性樹脂加工に用いられる、２本ロール、バンバリーミキサー、押出機、二軸混練押出機等が挙げられる。 The melt-kneading is preferably carried out at least at a temperature at which the thermoplastic elastomer (A), the mineral oil or the vegetable oil (B), and the resin component (C) are melted. As long as the mixing is performed by mechanical means, all kinds of mixing means are adopted, and typical means are stirring, mixing, and kneading, and the equipment having the function includes a stirrer, a mixer, and kneading. Machines, double rolls, Banbury mixers, extruders, twin-screw kneading extruders and the like used for rubber processing and thermoplastic resin processing can be mentioned.
混練工程は、熱可塑性エラストマー（Ａ）と鉱物系油または植物系油（Ｂ）とを予め添加した樹脂（マスターバッチ）に、樹脂成分（Ｃ）を添加して、二軸混錬押出機を用いて混練して、本発明の熱可塑性エラストマー組成物を得てもよい。なお、上記に記載した方法は混練工程の一例であり、単軸押出機を用いて熱可塑性エラストマー組成物の混練を行ってもよく、一般的に知られている分散剤を添加して熱可塑性エラストマー組成物の混練を行っても良い。 In the kneading step, the resin component (C) is added to the resin (masterbatch) to which the thermoplastic elastomer (A) and the mineral oil or the vegetable oil (B) are added in advance, and a twin-screw kneading extruder is used. It may be used and kneaded to obtain the thermoplastic elastomer composition of the present invention. The method described above is an example of a kneading step, and the thermoplastic elastomer composition may be kneaded using a uniaxial extruder, and a generally known dispersant may be added to make the thermoplastic elastomer composition. The elastomer composition may be kneaded.
＜熱可塑性エラストマー組成物の成形体＞
本発明にかかる熱可塑性エラストマー組成物の成形体は、混練工程と製膜工程からなる押出成形法、射出成形法、カレンダー成形法、ブロー成形法、圧縮成形法、など公知の方法により成形加工でき、成膜可能な膜厚範囲の広さから、押出成形法、射出成形法を好適に用いることができる。<Molded body of thermoplastic elastomer composition>
The molded body of the thermoplastic elastomer composition according to the present invention can be molded by a known method such as an extrusion molding method, an injection molding method, a calendar molding method, a blow molding method, a compression molding method, which comprises a kneading step and a film forming step. The extrusion molding method and the injection molding method can be preferably used because of the wide range of film thickness that can be formed.
本発明にかかる熱可塑性エラストマー組成物の成形体は、熱可塑性エラストマー組成物を成形用の金型に入れ、プレス機で加圧することにより作製できる（圧縮成形法）。熱可塑性エラストマー組成物を加圧する際に、金型に入れた熱可塑性エラストマー組成物を、軟化可能な温度に加熱すると、熱可塑性エラストマー組成物を所望の形状に加工しやすくなる。加圧工程を経た後、金型に入れた状態で熱可塑性エラストマー組成物の成形体を室温まで冷却して金型から取り出すと、熱可塑性エラストマー組成物の成形体が得られる。また、金型等を使用せずに、押出成形等により粒状物の成形体も製造することが出来る。 The molded product of the thermoplastic elastomer composition according to the present invention can be produced by placing the thermoplastic elastomer composition in a molding die and pressurizing it with a press machine (compression molding method). When the thermoplastic elastomer composition is pressed, if the thermoplastic elastomer composition placed in the mold is heated to a softable temperature, the thermoplastic elastomer composition can be easily processed into a desired shape. After undergoing the pressurizing step, the molded body of the thermoplastic elastomer composition is cooled to room temperature in a state of being placed in a mold and taken out from the mold to obtain a molded body of the thermoplastic elastomer composition. Further, it is possible to manufacture a granular molded product by extrusion molding or the like without using a mold or the like.
また、本発明にかかる熱可塑性エラストマー組成物の成形体は、混練工程で得られた熱可塑性エラストマー組成物を、押出機によりシート状に製膜することもできる。例えば、熱可塑性エラストマー組成物を、融点以上の温度（Ｔｍ〜Ｔｍ＋７０℃）に加熱された溶融押出機に供給して、熱可塑性エラストマー組成物を溶融し、製膜する。溶融押出機としては、一軸押出機、二軸押出機、ベント押出機、タンデム押出機等を目的に応じて使用することができる。 Further, in the molded body of the thermoplastic elastomer composition according to the present invention, the thermoplastic elastomer composition obtained in the kneading step can be formed into a sheet by an extruder. For example, the thermoplastic elastomer composition is supplied to a melt extruder heated to a temperature equal to or higher than the melting point (Tm to Tm + 70 ° C.) to melt the thermoplastic elastomer composition and form a film. As the melt extruder, a single-screw extruder, a twin-screw extruder, a vent extruder, a tandem extruder and the like can be used depending on the purpose.
また、本発明にかかる熱可塑性エラストマー組成物は、例えば、粒状体(ペレット等)として、加工することができる。熱可塑性エラストマーの粒状体の製造方法としては、例えば、混練工程で得られた熱可塑性エラストマー樹脂組成物を、一軸ルーダーにて溶融混練し、ストランドカットによりペレットを製造することができる。熱可塑性エラストマー組成物の粒状体の大きさは、０．１〜１０ｍｍの範囲が好ましい。 Further, the thermoplastic elastomer composition according to the present invention can be processed as, for example, granules (pellets or the like). As a method for producing the granular material of the thermoplastic elastomer, for example, the thermoplastic elastomer resin composition obtained in the kneading step can be melt-kneaded with a uniaxial luder, and pellets can be produced by strand cutting. The size of the granules of the thermoplastic elastomer composition is preferably in the range of 0.1 to 10 mm.
本発明の熱可塑性エラストマー組成物は、蓄熱材として好適に用いられるほか、自動車部品、家電部品、電線被覆、医療用部品、履物、雑貨、その他空調設備、建築材料、保温容器、保冷剤、コンクリート等にも用いることができる。たとえば、熱可塑性エラストマー組成物を成形加工することにより、、医療用シール部品、食品用シール部品、ボトルキャップパッキン、自動車用シール部品等の各種シール部材に好適に使用することができる。 The thermoplastic elastomer composition of the present invention is suitably used as a heat storage material, as well as automobile parts, home appliance parts, electric wire coatings, medical parts, footwear, miscellaneous goods, other air conditioning equipment, building materials, heat insulating containers, ice packs, concrete. It can also be used for. For example, by molding the thermoplastic elastomer composition, it can be suitably used for various sealing members such as medical sealing parts, food sealing parts, bottle cap packings, and automobile sealing parts.
本発明にかかる熱可塑性エラストマー組成物は、蓄熱材として各種の建材に使用することができる。建材用途に用いる熱可塑性エラストマー組成物は、鉱物系油または植物系油（Ｂ）が蓄熱材として使用可能な炭素数１４以上２０以下のｎ−パラフィンを５０質量％以上含むものであることが好ましい。熱可塑性エラストマー組成物は、石膏またはコンクリート等に混合することにより建材として使用することができる。 The thermoplastic elastomer composition according to the present invention can be used as a heat storage material in various building materials. The thermoplastic elastomer composition used for building materials preferably contains 50% by mass or more of n-paraffin having 14 or more and 20 or less carbon atoms in which the mineral oil or vegetable oil (B) can be used as a heat storage material. The thermoplastic elastomer composition can be used as a building material by mixing it with gypsum, concrete or the like.
本発明にかかる熱可塑性エラストマー組成物を建材用途に用いる場合、熱可塑性エラストマー組成物と建材との配合比は、５：９５〜８０：２０（質量比）とすることが好ましい。石膏ボードに用いる場合、熱可塑性エラストマー組成物と石膏等の配合比は、５：９５〜２０：８０とすることが強度の点で好ましい。 When the thermoplastic elastomer composition according to the present invention is used for building materials, the compounding ratio of the thermoplastic elastomer composition and the building material is preferably 5:95 to 80:20 (mass ratio). When used for gypsum board, the blending ratio of the thermoplastic elastomer composition and gypsum or the like is preferably 5:95 to 20:80 in terms of strength.
石膏ボード、石膏プラスター、石膏系セルフレベリング材に用いる場合、本発明の熱可塑性エラストマー組成物および半水石膏を主成分とする紛体原料に水分を添加し、撹拌してスラリー状組成物とし、施工または成形し、凝固、硬化させることにより製造することができる。石膏系の建材に使用する石膏原料としては、焼き石膏、硫酸カルシウム、を主成分とする鉱物（硫酸カルシウムの１／２水和物）である。 When used for gypsum board, gypsum plaster, and gypsum-based self-leveling material, water is added to the thermoplastic elastomer composition of the present invention and the powder raw material containing hemihydrate gypsum as the main component, and the mixture is stirred to form a slurry-like composition. Alternatively, it can be manufactured by molding, solidifying, and curing. The gypsum raw material used for gypsum-based building materials is a mineral (1/2 hydrate of calcium sulfate) containing calcined gypsum and calcium sulfate as main components.
また、本発明にかかる熱可塑性エラストマー組成物を石膏と混合して、塗り壁材としてもよい。例えば、本発明の熱可塑性エラストマー組成物、珪質頁岩粉粒物、焼き石膏、骨材、無機調整剤、水を混合し、均質なペーストになるまで混練し、塗り壁材を得ることができる。 Further, the thermoplastic elastomer composition according to the present invention may be mixed with gypsum to form a plaster wall material. For example, the thermoplastic elastomer composition of the present invention, siliceous shale granules, gypsum roast, aggregate, inorganic modifier, and water can be mixed and kneaded until a homogeneous paste is obtained to obtain a plastered wall material. ..
さらに、本発明にかかる熱可塑性エラストマー組成物を、接着剤と混合し、熱圧着することにより、集成材、パーティクルボード、ファイバーボード等の建材ボードとすることができる。
また、本発明にかかる熱可塑性エラストマー組成物を、小片（例えば、植物小片、植物繊維、木質繊維、木質チップ、竹小片、草小片等）および接着剤と混合し、熱圧着することにより、集成材、パーティクルボード、ファイバーボード等の建材ボードとすることもできる。Further, the thermoplastic elastomer composition according to the present invention is mixed with an adhesive and thermocompression bonded to obtain a building material board such as laminated wood, particle board, or fiber board.
Further, the thermoplastic elastomer composition according to the present invention is mixed with small pieces (for example, plant small pieces, plant fibers, wood fibers, wood chips, bamboo small pieces, grass small pieces, etc.) and an adhesive, and is assembled by thermocompression bonding. It can also be used as a building material board such as wood, particle board, or fiber board.
以下、実施例により本発明をさらに具体的に説明するが、本発明はこれらの実施例に限定されるものではない。 Hereinafter, the present invention will be described in more detail with reference to Examples, but the present invention is not limited to these Examples.
実施例および比較例で使用した各化学品は、市場から入手したものを、精製することなく使用した。以下、実施例および比較例に使用した熱可塑性エラストマー（Ａ）、鉱物系油または植物系油（Ｂ）、樹脂成分（Ｃ）および高級アルコール（Ｄ）を示す。 The chemicals used in the Examples and Comparative Examples were obtained from the market and used without purification. Hereinafter, the thermoplastic elastomer (A), the mineral oil or the vegetable oil (B), the resin component (C) and the higher alcohol (D) used in Examples and Comparative Examples are shown.
＜熱可塑性エラストマー（Ａ）＞
スチレン−エチレン／プロピレンブロック共重合体（ＳＥＰ）
クレイトンＧ１７０１ＥＵ （クレイトンポリマージャパン（株）製）
スチレン−エチレン／ブチレン−スチレンブロック共重合体（ＳＥＢＳ）
クレイトンＧ１６５１ＨＵ （クレイトンポリマージャパン（株）製）
エチレン−エチレン／共役ジエン−エチレンブロック共重合体（ＣＥＢＣ）
ダイナロン（登録商標）６３６０Ｂ （ＪＳＲ（株）製）<Thermoplastic elastomer (A)>
Styrene-Ethylene / Propylene Block Copolymer (SEP)
Kraton G1701EU (manufactured by Kraton Polymer Japan Co., Ltd.)
Styrene-Ethylene / Butylene-Styrene Block Copolymer (SEBS)
Kraton G1651HU (manufactured by Kraton Polymer Japan Co., Ltd.)
Ethylene-Ethylene / Conjugated Diene-Ethylene Block Copolymer (CEBC)
Dynaron (registered trademark) 6360B (manufactured by JSR Corporation)
＜鉱物系油または植物系油（Ｂ）＞
ｎ−ヘプタデカン（Ｃ１７）（ＪＸ日鉱日石エネルギー社製「ＴＳ−７（商品名）」）
ｎ−オクタデカン（Ｃ１８）（ＪＸ日鉱日石エネルギー社製「ＴＳ−８（商品名）」）<Mineral oil or vegetable oil (B)>
n-Heptadecane (C17) ("TS-7 (trade name)" manufactured by JX Nippon Oil Energy Co., Ltd.)
n-octadecane (C18) ("TS-8 (trade name)" manufactured by JX Nippon Oil Energy Co., Ltd.)
＜樹脂成分（Ｃ）＞
ホモプロピレンペレット（ＰＰ ＰＭ９００Ａ、サンアロマー（株）製）
ホモプロピレンペレット（ＰＰ ＰＬ４００Ａ、サンアロマー（株）製）
ランダムポリプロピレンペレット（ＰＰ ＰＢ２２２Ａ、サンアロマー（株）製）
ブロックポリプロピレンペレト（ＰＰ ＶＢ３７０Ａ、サンアロマー（株）製）
高密度ポリエチレン（ＨＤＰＥ ＨＦ５６０、日本ポリエチレン（株）製）
エチレン・酢酸ビニル共重合樹脂（ＥＶＡ ウルトラセン６２６、東ソー（株）製）
エチレン−プロピレン−ジエンゴム（ＥＰＤＭ ９０９０Ｍ、三井化学（株）製）
変性エチレン−プロピレンゴム（変性ＥＰＲ ＭＨ５０４０、三井化学（株）製）
＜高級アルコール（Ｄ）＞
ベヘニルアルコール（Ｃ２２） （東京化成工業（株）製）<Resin component (C)>
Homopropylene pellets (PP PM900A, manufactured by SunAllomer Ltd.)
Homopropylene pellets (PP PL400A, manufactured by SunAllomer Ltd.)
Random polypropylene pellets (PP PB222A, manufactured by SunAllomer Ltd.)
Block polypropylene peret (PP VB370A, manufactured by SunAllomer Ltd.)
High-density polyethylene (HDPE HF560, manufactured by Japan Polyethylene Corporation)
Ethylene-vinyl acetate copolymer resin (EVA Ultrasen 626, manufactured by Tosoh Corporation)
Ethylene-propylene-diene rubber (EPDM 9090M, manufactured by Mitsui Chemicals, Inc.)
Modified ethylene-propylene rubber (modified EPR MH5040, manufactured by Mitsui Chemicals, Inc.)
<Higher alcohol (D)>
Behenyl alcohol (C22) (manufactured by Tokyo Chemical Industry Co., Ltd.)
＜熱可塑性エラストマー組成物シートの製造＞
表１に示す種類および配合量の、鉱物系油または植物系油（Ｂ）と、熱可塑性エラストマー（Ａ）と、樹脂成分（Ｃ）とを混練押出機に投入し、選定樹脂の融点以上になるように加熱しつつ、５分間混練して熱可塑性エラストマー組成物を得た。そして熱可塑性エラストマー組成物を、シート形状の金型（成形サイズ１５０ｍｍ×１５０ｍｍ×２ｍｍ）に流し入れ、加熱プレス機を用いて金型温度が選定樹脂の融点以上となるように加熱しつつ、加圧成形した。加圧成形後、放冷し、金型から取り出したシート状の成形物から１５０ｍｍ×１５０ｍｍ×２ｍｍのシート状のサンプルを作成した。なお、実施例１、２では、鉱物系油または植物系油（Ｂ）として使用するｎ−ヘプタデカンとして、ベヘニルアルコール（高級アルコール（Ｄ））を１．２質量％の割合で添加したものを使用した。<Manufacturing of thermoplastic elastomer composition sheet>
The mineral oil or vegetable oil (B), the thermoplastic elastomer (A), and the resin component (C) of the types and blending amounts shown in Table 1 are put into a kneading extruder to exceed the melting point of the selected resin. The thermoplastic elastomer composition was obtained by kneading for 5 minutes while heating so as to become. Then, the thermoplastic elastomer composition is poured into a sheet-shaped mold (molding size 150 mm × 150 mm × 2 mm), and is pressurized while being heated so that the mold temperature becomes equal to or higher than the melting point of the selected resin using a heating press. Molded. After pressure molding, the mixture was allowed to cool, and a sheet-shaped sample of 150 mm × 150 mm × 2 mm was prepared from the sheet-shaped molded product taken out from the mold. In Examples 1 and 2, as the n-heptadecane used as the mineral oil or the vegetable oil (B), behenyl alcohol (higher alcohol (D)) was added at a ratio of 1.2% by mass. ..
＜熱可塑性エラストマー組成物ペレットの製造＞
表２および３に示す種類および配合量の、鉱物系油または植物系油（Ｂ）と、熱可塑性エラストマー（Ａ）と、樹脂成分（Ｃ）とを混練押出機に投入し、選定樹脂の融点以上になるように加熱しつつ、５分間混練して熱可塑性エラストマー組成物を得た。そして熱可塑性エラストマー組成物を、一軸ルーダーにて溶融混練し、ストランドカットにより平均粒径が約２ｍｍのペレットを得た。<Manufacturing of thermoplastic elastomer composition pellets>
The mineral oil or vegetable oil (B), the thermoplastic elastomer (A), and the resin component (C) of the types and blending amounts shown in Tables 2 and 3 are put into a kneading extruder, and the melting point of the selected resin is obtained. While heating as described above, the mixture was kneaded for 5 minutes to obtain a thermoplastic elastomer composition. Then, the thermoplastic elastomer composition was melt-kneaded with a uniaxial luder, and pellets having an average particle size of about 2 mm were obtained by strand cutting.
<ヒートサイクル試験１>
実施例１〜５、および比較例１〜３の処方で製造したシート状の熱可塑性エラストマー組成物（サイズ５０ｍｍ×５０ｍｍ×２ｍｍに切り出したもの）をポリエチレンフィルム（内層）とポリアミドフィルム（外層）とからなる積層フィルムにて包装してヒートサイクル試験サンプルとした。各熱可塑性エラストマー組成物が含有する鉱物系油または植物系油（Ｂ）の融点に対し、−５〜−１５℃以下の範囲にある恒温槽Ａ、および、＋５〜＋１５℃以上の範囲にある恒温槽Ｂを用意し、評価試料を恒温槽Ａ、Ｂに交互に浸漬して、熱可塑性エラストマー組成物の相転移を５０回繰り返した後、相分離の有無を評価した。ヒートサイクル試験は、評価試料を融点より低い温度とした恒温槽Ａに浸漬し、熱可塑性エラストマー組成物中の鉱物系油または植物系油（Ｂ）の凝固・固化相転移を目視により確認した後（組成物全体の白濁化）、融点より高い温度とした恒温槽Ｂに評価試料を浸漬し、熱可塑性エラストマー組成物中の鉱物系油または植物系油（Ｂ）の溶解・液化相転移を目視により確認（組成物全体の半透明化）すること（固化および液化を各１回）を繰り返し（５０回）行った。ヒートサイクル５０回後に鉱物系油または植物系油（Ｂ）がブリードアウト（相分離発生）しないものを「○」、５０回未満でブリードアウト（相分離発生）したものを「×」と評価した。なお、両恒温槽の温度差は、概ね、１５℃〜３０℃の範囲である。結果を表１に示す。<Heat cycle test 1>
Sheet-shaped thermoplastic elastomer compositions (cut out to a size of 50 mm × 50 mm × 2 mm) produced by the formulations of Examples 1 to 5 and Comparative Examples 1 to 3 were combined with a polyethylene film (inner layer) and a polyamide film (outer layer). It was wrapped in a laminated film made of a heat cycle test sample. With respect to the melting point of the mineral oil or vegetable oil (B) contained in each thermoplastic elastomer composition, the constant temperature bath A in the range of -5 to -15 ° C or lower and the constant temperature bath A in the range of +5 to + 15 ° C or higher. A constant temperature bath B was prepared, the evaluation samples were alternately immersed in the constant temperature baths A and B, the phase transition of the thermoplastic elastomer composition was repeated 50 times, and then the presence or absence of phase separation was evaluated. In the heat cycle test, the evaluation sample is immersed in a constant temperature bath A having a temperature lower than the melting point, and the solidification / solidification phase transition of the mineral oil or the vegetable oil (B) in the thermoplastic elastomer composition is visually confirmed. (Whitening of the entire composition), Immerse the evaluation sample in a constant temperature bath B at a temperature higher than the melting point, and visually observe the dissolution / liquefaction phase transition of the mineral oil or vegetable oil (B) in the thermoplastic elastomer composition. Confirmation (translucency of the entire composition) (solidification and liquefaction once each) was repeated (50 times). Those in which the mineral oil or vegetable oil (B) did not bleed out (phase separation occurred) after 50 heat cycles were evaluated as "○", and those in which bleed out (phase separation occurred) in less than 50 times were evaluated as "x". .. The temperature difference between the two constant temperature baths is generally in the range of 15 ° C. to 30 ° C. The results are shown in Table 1.
<ヒートサイクル試験２>
ペレット状の熱可塑性エラストマー組成物１ｇを載置した金属シャーレを、恒温槽内で加熱および冷却する。加熱および冷却条件は、開始温度２０℃から０．２５℃／分で３０℃まで昇温して６０分間保持した後、０．２５℃／分で２０℃まで冷却して６０分保持する。この加熱および冷却工程を３回繰り返した後、熱可塑性エラストマー組成物の質量を秤量した。<Heat cycle test 2>
A metal petri dish on which 1 g of a pelletized thermoplastic elastomer composition is placed is heated and cooled in a constant temperature bath. The heating and cooling conditions are such that the temperature is raised from 20 ° C. to 0.25 ° C./min to 30 ° C. and held for 60 minutes, then cooled to 20 ° C. at 0.25 ° C./min and held for 60 minutes. After repeating this heating and cooling step three times, the mass of the thermoplastic elastomer composition was weighed.
＜凝固開始温度および凝固熱量＞
凝固開始温度および凝固熱量は示差熱熱量計（米国パーキンエルマー社製、ＤＳＣ−７型）を用いて測定した。<Coagulation start temperature and heat of solidification>
The solidification start temperature and the amount of heat of solidification were measured using a differential calorimeter (DSC-7 type manufactured by PerkinElmer, USA).
＜海島構造の島相の面積割合＞
ウルトラミクロトーム（Leica製 ULTRACUT−S）で熱可塑性エラストマー組成物の超薄切片を作製し、透過電子顕微鏡（以下、TEMと記する）で観察した。その観察したTEM画像の解析から、海島構造の島部分が視野に占める面積率を測定した。
〈TEM観察条件〉
装置名：透過電子顕微鏡 日立製作所製 H-800
加速電圧：200kV
染色処理：RuO4
〈画像解析による面積率測定〉
装置名：高速画像処理装置 カールツァイス製 AxioVision
測定項目：海島構造の島部分の面積率
測定条件：TEM画像を紙に印刷し、OHPシート（透明なプラシート）をかぶせて島部をトレースした。
得られたOHPトレースしたものを画像解析装置に入力し、その面積を求めた。その求めた面積を視野面積（410.1μｍ２）で除して面積率とした。<Area ratio of island fauna of sea island structure>
An ultrathin section of the thermoplastic elastomer composition was prepared with an ultramicrotome (ULTRACUT-S manufactured by Leica) and observed with a transmission electron microscope (hereinafter referred to as TEM). From the analysis of the observed TEM image, the area ratio of the island part of the sea island structure to the field of view was measured.
<TEM observation conditions>
Device name: Transmission electron microscope Hitachi, Ltd. H-800
Acceleration voltage: 200kV
Dyeing process: RuO4
<Measurement of area ratio by image analysis>
Device name: High-speed image processing device Carl Zeiss AxioVision
Measurement item: Area ratio of island part of sea island structure Measurement condition: TEM image was printed on paper and covered with OHP sheet (transparent plastic sheet) to trace the island part.
The obtained OHP trace was input to the image analyzer, and the area was calculated. The obtained area was divided by the visual field area (410.1 μm 2 ) to obtain the area ratio.
熱可塑性エラストマー（Ａ）として、分子中にポリスチレンブロックを１つのみ有するＳＥＰを使用した実施例１〜５では、ヒートサイクル試験においてブリードが見られなかった。これに対し、分子中にポリスチレンブロックを２つ有するＳＥＢＳおよびＳＥＰＳを使用した比較例１および２では、ヒートサイクル試験においてブリードが確認された。また、分子中にポリエチレンブロックを含まないＳＥＰを使用した実施例３は、ポリエチレンブロックを含むＳＥＢＳを使用した比較例１より高い凝固熱量が得られた。 No bleeding was observed in the heat cycle test in Examples 1 to 5 in which SEP having only one polystyrene block in the molecule was used as the thermoplastic elastomer (A). On the other hand, in Comparative Examples 1 and 2 using SEBS and SEPS having two polystyrene blocks in the molecule, bleeding was confirmed in the heat cycle test. Further, in Example 3 in which SEP containing no polyethylene block in the molecule was used, a higher amount of heat of solidification was obtained than in Comparative Example 1 in which SEBS containing a polyethylene block was used.
また、熱可塑性エラストマー（Ａ）、鉱物系油または植物系油（Ｂ）および樹脂成分（Ｃ）の配合量を変更した実施例３、実施例６〜１２より、樹脂成分（Ｃ）の割合が３５質量％以上の場合、急激に島相の面積割合が低下し、凝固熱量も低下することが確認できた。 Further, from Examples 3 and 6 to 12 in which the blending amounts of the thermoplastic elastomer (A), the mineral oil or the vegetable oil (B) and the resin component (C) were changed, the ratio of the resin component (C) was higher. When it was 35% by mass or more, it was confirmed that the area ratio of the island phase decreased sharply and the amount of heat of solidification also decreased.
また、図１、図３および図４より、熱可塑性エラストマー（Ａ）の配合割合が上昇すると（樹脂成分（Ｃ）の配合割合が低下）、海島構造の相分離構造（構造周期）が小さくなり、分散状態の安定化が確認された。 Further, from FIGS. 1, 3 and 4, as the compounding ratio of the thermoplastic elastomer (A) increases (the compounding ratio of the resin component (C) decreases), the phase-separated structure (structural period) of the sea-island structure becomes smaller. , The stabilization of the dispersed state was confirmed.
本発明の熱可塑性エラストマー組成物、および成形体は、建材、自動車部品、家電部品、電線被覆、医療用部品に有用であり、特に、発生する熱を吸熱して温度変化を抑制する用途、例えば、住宅等の内材、建築材や、自動車などの空調用途等において好適である。 The thermoplastic elastomer composition and molded article of the present invention are useful for building materials, automobile parts, home electric appliance parts, electric wire coatings, and medical parts, and in particular, applications for absorbing generated heat and suppressing temperature changes, for example. It is suitable for internal materials such as houses, building materials, and air conditioning applications such as automobiles.
Claims (17)
芳香族炭化水素、ナフテン系炭化水素およびパラフィン系炭化水素の混合物であって、該混合物中の成分のうち、ナフテン系炭化水素またはパラフィン系炭化水素の割合が最大である鉱物系油、またはパラフィン系炭化水素からなる植物系油（Ｂ）と、
樹脂成分（Ｃ）と、を含むことを特徴とする蓄熱材組成物。 Thermoplastic elastomer (A) having only one polystyrene block in the molecule,
A mixture of aromatic hydrocarbons, naphthenic hydrocarbons and paraffinic hydrocarbons, which is a mineral oil or paraffinic oil having the largest proportion of naphthenic hydrocarbons or paraffinic hydrocarbons among the components in the mixture. Vegetable oil (B) composed of hydrocarbons and
A heat storage material composition comprising a resin component (C).
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