TW201527380A - Heat-curable resin composition for optical semiconductor device, lead frame for optical semiconductor device and obtained using same, and optical semiconductor device - Google Patents
Heat-curable resin composition for optical semiconductor device, lead frame for optical semiconductor device and obtained using same, and optical semiconductor device Download PDFInfo
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- TW201527380A TW201527380A TW103140781A TW103140781A TW201527380A TW 201527380 A TW201527380 A TW 201527380A TW 103140781 A TW103140781 A TW 103140781A TW 103140781 A TW103140781 A TW 103140781A TW 201527380 A TW201527380 A TW 201527380A
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- Prior art keywords
- optical semiconductor
- semiconductor device
- reflector
- lead frame
- resin composition
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- 239000004065 semiconductor Substances 0.000 title claims abstract description 117
- 230000003287 optical effect Effects 0.000 title claims abstract description 111
- 239000011342 resin composition Substances 0.000 title claims abstract description 54
- 229920005989 resin Polymers 0.000 claims abstract description 32
- 239000011347 resin Substances 0.000 claims abstract description 32
- 239000000463 material Substances 0.000 claims abstract description 20
- 239000012463 white pigment Substances 0.000 claims abstract description 17
- 229920001187 thermosetting polymer Polymers 0.000 claims description 67
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 32
- 239000011256 inorganic filler Substances 0.000 claims description 12
- 229910003475 inorganic filler Inorganic materials 0.000 claims description 12
- 238000001721 transfer moulding Methods 0.000 claims description 10
- 229920002050 silicone resin Polymers 0.000 claims description 6
- 238000011068 loading method Methods 0.000 claims description 3
- 238000001746 injection moulding Methods 0.000 claims description 2
- 229910052751 metal Inorganic materials 0.000 abstract description 27
- 239000002184 metal Substances 0.000 abstract description 27
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 abstract description 2
- 229910001928 zirconium oxide Inorganic materials 0.000 abstract description 2
- 239000003822 epoxy resin Substances 0.000 description 37
- 229920000647 polyepoxide Polymers 0.000 description 37
- 238000001723 curing Methods 0.000 description 32
- 239000003795 chemical substances by application Substances 0.000 description 31
- 239000003054 catalyst Substances 0.000 description 24
- -1 bisphenol Chemical compound 0.000 description 20
- LNOLJFCCYQZFBQ-BUHFOSPRSA-N (ne)-n-[(4-nitrophenyl)-phenylmethylidene]hydroxylamine Chemical compound C=1C=C([N+]([O-])=O)C=CC=1C(=N/O)/C1=CC=CC=C1 LNOLJFCCYQZFBQ-BUHFOSPRSA-N 0.000 description 18
- DIOQZVSQGTUSAI-UHFFFAOYSA-N decane Chemical compound CCCCCCCCCC DIOQZVSQGTUSAI-UHFFFAOYSA-N 0.000 description 18
- 238000006482 condensation reaction Methods 0.000 description 15
- 150000008064 anhydrides Chemical class 0.000 description 14
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 13
- 238000005984 hydrogenation reaction Methods 0.000 description 12
- 239000002245 particle Substances 0.000 description 12
- 239000000843 powder Substances 0.000 description 12
- OAKJQQAXSVQMHS-UHFFFAOYSA-N Hydrazine Chemical compound NN OAKJQQAXSVQMHS-UHFFFAOYSA-N 0.000 description 10
- 238000007259 addition reaction Methods 0.000 description 9
- 239000007788 liquid Substances 0.000 description 9
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 8
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 8
- 238000006243 chemical reaction Methods 0.000 description 8
- 229930195735 unsaturated hydrocarbon Natural products 0.000 description 8
- 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 7
- 239000004848 polyfunctional curative Substances 0.000 description 7
- 229910052707 ruthenium Inorganic materials 0.000 description 7
- 238000007789 sealing Methods 0.000 description 7
- 239000004593 Epoxy Substances 0.000 description 6
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 6
- MWPLVEDNUUSJAV-UHFFFAOYSA-N anthracene Chemical compound C1=CC=CC2=CC3=CC=CC=C3C=C21 MWPLVEDNUUSJAV-UHFFFAOYSA-N 0.000 description 6
- 229910010293 ceramic material Inorganic materials 0.000 description 6
- 150000002430 hydrocarbons Chemical group 0.000 description 6
- 229910052697 platinum Inorganic materials 0.000 description 6
- 239000000126 substance Substances 0.000 description 6
- 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 5
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 5
- 239000002253 acid Substances 0.000 description 5
- 229910000420 cerium oxide Inorganic materials 0.000 description 5
- 238000009833 condensation Methods 0.000 description 5
- 230000005494 condensation Effects 0.000 description 5
- 150000007973 cyanuric acids Chemical class 0.000 description 5
- MWKFXSUHUHTGQN-UHFFFAOYSA-N decan-1-ol Chemical compound CCCCCCCCCCO MWKFXSUHUHTGQN-UHFFFAOYSA-N 0.000 description 5
- 239000003063 flame retardant Substances 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 5
- 150000003304 ruthenium compounds Chemical class 0.000 description 5
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 5
- MUTGBJKUEZFXGO-OLQVQODUSA-N (3as,7ar)-3a,4,5,6,7,7a-hexahydro-2-benzofuran-1,3-dione Chemical compound C1CCC[C@@H]2C(=O)OC(=O)[C@@H]21 MUTGBJKUEZFXGO-OLQVQODUSA-N 0.000 description 4
- FKBMTBAXDISZGN-UHFFFAOYSA-N 5-methyl-3a,4,5,6,7,7a-hexahydro-2-benzofuran-1,3-dione Chemical compound C1C(C)CCC2C(=O)OC(=O)C12 FKBMTBAXDISZGN-UHFFFAOYSA-N 0.000 description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 150000001875 compounds Chemical class 0.000 description 4
- 239000001257 hydrogen Substances 0.000 description 4
- 229910052739 hydrogen Inorganic materials 0.000 description 4
- 238000004898 kneading Methods 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 238000000465 moulding Methods 0.000 description 4
- 229910052698 phosphorus Inorganic materials 0.000 description 4
- 239000011574 phosphorus Substances 0.000 description 4
- 239000000758 substrate Substances 0.000 description 4
- 239000011787 zinc oxide Substances 0.000 description 4
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 3
- LGRFSURHDFAFJT-UHFFFAOYSA-N Phthalic anhydride Natural products C1=CC=C2C(=O)OC(=O)C2=C1 LGRFSURHDFAFJT-UHFFFAOYSA-N 0.000 description 3
- 239000007983 Tris buffer Substances 0.000 description 3
- 239000000654 additive Substances 0.000 description 3
- 125000002723 alicyclic group Chemical group 0.000 description 3
- 125000001931 aliphatic group Chemical group 0.000 description 3
- 125000003342 alkenyl group Chemical group 0.000 description 3
- 125000000217 alkyl group Chemical group 0.000 description 3
- 239000002518 antifoaming agent Substances 0.000 description 3
- JHIWVOJDXOSYLW-UHFFFAOYSA-N butyl 2,2-difluorocyclopropane-1-carboxylate Chemical compound CCCCOC(=O)C1CC1(F)F JHIWVOJDXOSYLW-UHFFFAOYSA-N 0.000 description 3
- 239000007822 coupling agent Substances 0.000 description 3
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 3
- RAXXELZNTBOGNW-UHFFFAOYSA-N imidazole Natural products C1=CNC=N1 RAXXELZNTBOGNW-UHFFFAOYSA-N 0.000 description 3
- 239000012948 isocyanate Substances 0.000 description 3
- 150000002513 isocyanates Chemical class 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- 150000002923 oximes Chemical group 0.000 description 3
- 229910052723 transition metal Inorganic materials 0.000 description 3
- 150000003624 transition metals Chemical class 0.000 description 3
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 3
- KMOUUZVZFBCRAM-OLQVQODUSA-N (3as,7ar)-3a,4,7,7a-tetrahydro-2-benzofuran-1,3-dione Chemical compound C1C=CC[C@@H]2C(=O)OC(=O)[C@@H]21 KMOUUZVZFBCRAM-OLQVQODUSA-N 0.000 description 2
- OUPZKGBUJRBPGC-UHFFFAOYSA-N 1,3,5-tris(oxiran-2-ylmethyl)-1,3,5-triazinane-2,4,6-trione Chemical compound O=C1N(CC2OC2)C(=O)N(CC2OC2)C(=O)N1CC1CO1 OUPZKGBUJRBPGC-UHFFFAOYSA-N 0.000 description 2
- KBPLFHHGFOOTCA-UHFFFAOYSA-N 1-Octanol Chemical compound CCCCCCCCO KBPLFHHGFOOTCA-UHFFFAOYSA-N 0.000 description 2
- GQHTUMJGOHRCHB-UHFFFAOYSA-N 2,3,4,6,7,8,9,10-octahydropyrimido[1,2-a]azepine Chemical compound C1CCCCN2CCCN=C21 GQHTUMJGOHRCHB-UHFFFAOYSA-N 0.000 description 2
- MFAWEYJGIGIYFH-UHFFFAOYSA-N 2-[4-(trimethoxymethyl)dodecoxymethyl]oxirane Chemical compound C(C1CO1)OCCCC(C(OC)(OC)OC)CCCCCCCC MFAWEYJGIGIYFH-UHFFFAOYSA-N 0.000 description 2
- QXBYUPMEYVDXIQ-UHFFFAOYSA-N 4-methyl-3a,4,5,6,7,7a-hexahydro-2-benzofuran-1,3-dione Chemical compound CC1CCCC2C(=O)OC(=O)C12 QXBYUPMEYVDXIQ-UHFFFAOYSA-N 0.000 description 2
- RMDKEBZUCHXUER-UHFFFAOYSA-N 4-methylbicyclo[2.2.1]hept-2-ene Chemical compound C1CC2C=CC1(C)C2 RMDKEBZUCHXUER-UHFFFAOYSA-N 0.000 description 2
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- QIGBRXMKCJKVMJ-UHFFFAOYSA-N Hydroquinone Chemical compound OC1=CC=C(O)C=C1 QIGBRXMKCJKVMJ-UHFFFAOYSA-N 0.000 description 2
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- 150000001335 aliphatic alkanes Chemical class 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- ADCOVFLJGNWWNZ-UHFFFAOYSA-N antimony trioxide Chemical compound O=[Sb]O[Sb]=O ADCOVFLJGNWWNZ-UHFFFAOYSA-N 0.000 description 2
- 239000003963 antioxidant agent Substances 0.000 description 2
- 230000003078 antioxidant effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical class C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 2
- 239000004841 bisphenol A epoxy resin Substances 0.000 description 2
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- 239000000919 ceramic Substances 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 239000004205 dimethyl polysiloxane Substances 0.000 description 2
- 235000013870 dimethyl polysiloxane Nutrition 0.000 description 2
- ZUOUZKKEUPVFJK-UHFFFAOYSA-N diphenyl Chemical compound C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 description 2
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- 239000003112 inhibitor Substances 0.000 description 2
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- JFNLZVQOOSMTJK-KNVOCYPGSA-N norbornene Chemical compound C1[C@@H]2CC[C@H]1C=C2 JFNLZVQOOSMTJK-KNVOCYPGSA-N 0.000 description 2
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- 229920002554 vinyl polymer Polymers 0.000 description 2
- DQGPWNBGAYGUPK-UHFFFAOYSA-N 1,1,1-trifluoro-4-(trimethoxymethyl)dodecane Chemical compound FC(CCC(C(OC)(OC)OC)CCCCCCCC)(F)F DQGPWNBGAYGUPK-UHFFFAOYSA-N 0.000 description 1
- ANBBCZAIOXDZPV-UHFFFAOYSA-N 1,1,1-trimethoxy-2-methyldecane Chemical compound CC(C(OC)(OC)OC)CCCCCCCC ANBBCZAIOXDZPV-UHFFFAOYSA-N 0.000 description 1
- QIKSEZYONUMDRR-UHFFFAOYSA-N 1,3-dioxo-3a,4,5,6,7,7a-hexahydro-2-benzofuran-4,5-dicarboxylic acid Chemical compound OC(=O)C1C(C(=O)O)CCC2C(=O)OC(=O)C12 QIKSEZYONUMDRR-UHFFFAOYSA-N 0.000 description 1
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- YTPFRRRNIYVFFE-UHFFFAOYSA-N 2,2,3,3,5,5-hexamethyl-1,4-dioxane Chemical compound CC1(C)COC(C)(C)C(C)(C)O1 YTPFRRRNIYVFFE-UHFFFAOYSA-N 0.000 description 1
- GCZWJRLXIPVNLU-UHFFFAOYSA-N 2,2-dimethoxy-3-methylundecane Chemical compound CC(C(OC)(OC)C)CCCCCCCC GCZWJRLXIPVNLU-UHFFFAOYSA-N 0.000 description 1
- FALRKNHUBBKYCC-UHFFFAOYSA-N 2-(chloromethyl)pyridine-3-carbonitrile Chemical compound ClCC1=NC=CC=C1C#N FALRKNHUBBKYCC-UHFFFAOYSA-N 0.000 description 1
- LXBGSDVWAMZHDD-UHFFFAOYSA-N 2-methyl-1h-imidazole Chemical compound CC1=NC=CN1 LXBGSDVWAMZHDD-UHFFFAOYSA-N 0.000 description 1
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- LARNQUAWIRVQPK-UHFFFAOYSA-N 2-methyloxiran-2-amine Chemical compound NC1(CO1)C LARNQUAWIRVQPK-UHFFFAOYSA-N 0.000 description 1
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- PAVNZLVXYJDFNR-UHFFFAOYSA-N 3,3-dimethyloxane-2,6-dione Chemical compound CC1(C)CCC(=O)OC1=O PAVNZLVXYJDFNR-UHFFFAOYSA-N 0.000 description 1
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- DFYGYTNMHPUJBY-UHFFFAOYSA-N 4-(trimethoxymethyl)dodecane-1-thiol Chemical compound SCCCC(C(OC)(OC)OC)CCCCCCCC DFYGYTNMHPUJBY-UHFFFAOYSA-N 0.000 description 1
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- SRITWFDREMKSQQ-UHFFFAOYSA-N [Pt].C(=C)C1(C(OC(C(O1)C)C)(C)C=C)C Chemical compound [Pt].C(=C)C1(C(OC(C(O1)C)C)(C)C=C)C SRITWFDREMKSQQ-UHFFFAOYSA-N 0.000 description 1
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
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- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
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- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 238000001579 optical reflectometry Methods 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 150000002898 organic sulfur compounds Chemical class 0.000 description 1
- 229920006136 organohydrogenpolysiloxane Polymers 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
- DYFXGORUJGZJCA-UHFFFAOYSA-N phenylmethanediamine Chemical compound NC(N)C1=CC=CC=C1 DYFXGORUJGZJCA-UHFFFAOYSA-N 0.000 description 1
- 150000003018 phosphorus compounds Chemical class 0.000 description 1
- 150000003057 platinum Chemical class 0.000 description 1
- 150000003058 platinum compounds Chemical class 0.000 description 1
- 229920000768 polyamine Polymers 0.000 description 1
- 230000019617 pupation Effects 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000012552 review Methods 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 239000010948 rhodium Substances 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000007858 starting material 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
- 229940014800 succinic anhydride Drugs 0.000 description 1
- 239000000454 talc Substances 0.000 description 1
- 229910052623 talc Inorganic materials 0.000 description 1
- 150000003512 tertiary amines Chemical class 0.000 description 1
- UFDHBDMSHIXOKF-UHFFFAOYSA-N tetrahydrophthalic acid Natural products OC(=O)C1=C(C(O)=O)CCCC1 UFDHBDMSHIXOKF-UHFFFAOYSA-N 0.000 description 1
- QEMXHQIAXOOASZ-UHFFFAOYSA-N tetramethylammonium Chemical class C[N+](C)(C)C QEMXHQIAXOOASZ-UHFFFAOYSA-N 0.000 description 1
- BRKFQVAOMSWFDU-UHFFFAOYSA-M tetraphenylphosphanium;bromide Chemical compound [Br-].C1=CC=CC=C1[P+](C=1C=CC=CC=1)(C=1C=CC=CC=1)C1=CC=CC=C1 BRKFQVAOMSWFDU-UHFFFAOYSA-M 0.000 description 1
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- HXMCVXVDQLXIKI-UHFFFAOYSA-K tributyl(methyl)phosphanium phosphate Chemical compound P(=O)([O-])([O-])[O-].C[P+](CCCC)(CCCC)CCCC.C[P+](CCCC)(CCCC)CCCC.C[P+](CCCC)(CCCC)CCCC HXMCVXVDQLXIKI-UHFFFAOYSA-K 0.000 description 1
- SRPWOOOHEPICQU-UHFFFAOYSA-N trimellitic anhydride Chemical compound OC(=O)C1=CC=C2C(=O)OC(=O)C2=C1 SRPWOOOHEPICQU-UHFFFAOYSA-N 0.000 description 1
- 239000006097 ultraviolet radiation absorber Substances 0.000 description 1
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000010969 white metal Substances 0.000 description 1
Classifications
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- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
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- H01L24/00—Arrangements for connecting or disconnecting semiconductor or solid-state bodies; Methods or apparatus related thereto
- H01L24/93—Batch processes
- H01L24/95—Batch processes at chip-level, i.e. with connecting carried out on a plurality of singulated devices, i.e. on diced chips
- H01L24/97—Batch processes at chip-level, i.e. with connecting carried out on a plurality of singulated devices, i.e. on diced chips the devices being connected to a common substrate, e.g. interposer, said common substrate being separable into individual assemblies after connecting
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- H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
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- H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
- H01L33/62—Arrangements for conducting electric current to or from the semiconductor body, e.g. lead-frames, wire-bonds or solder balls
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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- H01L2224/48257—Connecting between a semiconductor or solid-state body and an item not being a semiconductor or solid-state body, e.g. chip-to-substrate, chip-to-passive the body and the item being stacked the item being metallic connecting the wire to a die pad of the item
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Abstract
Description
本發明是有關於作為反射器(反射部)形成材料的光半導體裝置用熱硬化性樹脂組成物及使用其而得之光半導體裝置用引線框、以及光半導體裝置，前述反射器是用以使由發光元件發出之波長350~410nm的光反射。 The present invention relates to a thermosetting resin composition for an optical semiconductor device which is a material for forming a reflector (reflecting portion), a lead frame for an optical semiconductor device using the same, and an optical semiconductor device, wherein the reflector is used for Light emitted by a light-emitting element having a wavelength of 350 to 410 nm is reflected.
以往，在裝載發出紫外線(UV)範圍之光的發光元件而成的光半導體裝置中，作為用以使由該發光元件發出之光反射的反射器，一直以來均使用陶瓷材料。 Conventionally, in an optical semiconductor device in which a light-emitting element that emits light in an ultraviolet (UV) range is mounted, a ceramic material has been conventionally used as a reflector for reflecting light emitted from the light-emitting element.
另一方面，在這類光半導體裝置中，裝載發出如上述UV範圍之特定波長範圍之光的發光元件以外之發光元件而成的光半導體裝置，近年來則使用以環氧樹脂等為代表之熱硬化性樹脂，藉由例如轉移成形(transfer molding)等成形製造上述反射器。並且，上述熱硬化性樹脂中一直是摻混氧化鈦作為白色顏料，以反射由上述光半導體元件發出之光(參照專利文獻1)。 On the other hand, in such an optical semiconductor device, an optical semiconductor device in which a light-emitting element other than a light-emitting element that emits light in a specific wavelength range of the above-described UV range is mounted is represented by an epoxy resin or the like. The thermosetting resin is produced by molding such a reflector by, for example, transfer molding. In the thermosetting resin, titanium oxide is blended as a white pigment to reflect light emitted from the optical semiconductor element (see Patent Document 1).
專利文獻1：日本專利特開2011-258845號公報 Patent Document 1: Japanese Patent Laid-Open No. 2011-258845
裝載發出如上述UV範圍之特定波長範圍之光的發光元件而成的光半導體裝置中，將摻混有氧化鈦作為白色顏料之熱硬化性樹脂用作反射器材料時，會產生對上述光的光反射率降低、且因光致變色(photochromism)而著色成暗藍色的問題，因此如前所述，反射器材料僅使用陶瓷。 In an optical semiconductor device in which a light-emitting element that emits light of a specific wavelength range of the above-described UV range is used, when a thermosetting resin in which titanium oxide is used as a white pigment is used as a reflector material, light is generated. Since the light reflectance is lowered and the color is dark blue due to photochromism, as described above, only the ceramic is used as the reflector material.
但是，如上述使用陶瓷來作為UV範圍反射器材料時，從其材料特性而言顯然難以賦予各種形狀，而且由上述陶瓷材料構成之反射器通常對上述波長範圍之光的光反射率並未超過90%，所以對於可取代陶瓷材料之反射器材料、特別是可以透過各種成形方法製作成各種形狀之有機系反射器材料，抱有很強烈的期待。 However, when ceramic is used as the UV range reflector material as described above, it is apparent that it is difficult to impart various shapes from the material properties thereof, and the reflector composed of the above ceramic material generally does not exceed the light reflectance of light in the above wavelength range. Since it is 90%, there is a strong expectation for a reflector material which can replace a ceramic material, in particular, an organic reflector material which can be produced into various shapes by various molding methods.
本發明是有鑒於上述情形而起，其目的在於提供一種光半導體裝置用熱硬化性樹脂組成物及使用其而得之光半導體裝置用引線框、以及光半導體裝置，且前述光半導體裝置用熱硬化性樹脂組成物為可對350~410nm之特定波長範圍發揮高的光反射率、且可輕易形成各種形狀的有機系材料。 In view of the above, it is an object of the present invention to provide a thermosetting resin composition for an optical semiconductor device, a lead frame for an optical semiconductor device using the same, and an optical semiconductor device, and the heat of the optical semiconductor device The curable resin composition is an organic material which can exhibit a high light reflectance in a specific wavelength range of 350 to 410 nm and can easily form various shapes.
為了達成上述目的，本發明以光半導體裝置用熱 硬化性樹脂組成物為第1要旨，該光半導體裝置用熱硬化性樹脂組成物是作為具備波長350~410nm之發光元件之光半導體裝置的反射器形成材料來使用，並含有下述(A)及(B)：(A)熱硬化性樹脂；(B)僅由氧化鋯形成之白色顏料。 In order to achieve the above object, the present invention uses heat for an optical semiconductor device In the first aspect of the invention, the thermosetting resin composition for an optical semiconductor device is used as a reflector forming material for an optical semiconductor device having a light-emitting element having a wavelength of 350 to 410 nm, and contains the following (A). And (B): (A) a thermosetting resin; (B) a white pigment formed only of zirconia.
並且，本發明以光半導體裝置用引線框為第2要旨，該光半導體裝置用引線框是用以僅在厚度方向的一面上裝載光半導體元件之板狀光半導體裝置用引線框，其乃具備互相隔著間隙配置之多數個板部，並在上述間隙中形成反射器而成，且該反射器是使用上述第1要旨之光半導體裝置用熱硬化性樹脂組成物填充於上述間隙中並經硬化而成。又，本發明以光半導體裝置用引線框為第3要旨，該光半導體裝置用引線框是具備光半導體元件裝載區域並形成反射器而成的立體狀光半導體裝置用引線框，且該反射器是呈以其本身之至少一部分包圍元件裝載區域周圍之狀態形成；又，上述反射器是使用上述第1要旨之光半導體裝置用熱硬化性樹脂組成物形成而成。 Further, the present invention is directed to a lead frame for an optical semiconductor device, which is a lead frame for a plate-shaped optical semiconductor device in which an optical semiconductor element is mounted on only one surface in a thickness direction, and is provided with a lead frame for an optical semiconductor device. a plurality of plate portions disposed with a gap therebetween, and a reflector is formed in the gap, and the reflector is filled in the gap by a thermosetting resin composition for an optical semiconductor device according to the first aspect. Hardened. In the third aspect of the present invention, a lead frame for an optical semiconductor device is a lead frame for a three-dimensional optical semiconductor device including a photo-semiconductor mounting region and a reflector, and the reflector is provided. The reflector is formed in a state in which at least a part of the component is surrounded by the component mounting region, and the reflector is formed of a thermosetting resin composition for an optical semiconductor device according to the first aspect.
此外，本發明以光半導體裝置為第4要旨，該光半導體裝置係使於其一面上具有用以裝載發光元件之元件搭載區域的板部互相隔著間隙配置，且在上述元件裝載區域之預定位置上裝載350~410nm的發光元件而成者；又，該光半導裝置是在上述間隙中形成反射器而成，且該反射器是使用上述第1要旨之半導體裝置用熱硬化性樹脂組成物填充於上述間隙中並經硬化而成。又，本發明以光半導 體裝置為第5要旨，該光半導體裝置係在光半導體裝置用引線框之預定位置上裝載波長350~410nm的發光元件而成者，該光半導體裝置用引線框係具備發光元件裝載區域並形成反射器而成，且該反射器是呈以其本身之至少一部分包圍元件裝載區域周圍之狀態形成；又，上述反射器是使用上述第1要旨之光半導體裝置用熱硬化性樹脂組成物形成而成。 Further, the present invention is directed to an optical semiconductor device in which a plate portion having an element mounting region on which a light-emitting element is mounted is disposed with a gap therebetween, and is predetermined in the component loading region. A light-emitting element of 350 to 410 nm is mounted at a position; and the light-guiding device is formed by forming a reflector in the gap, and the reflector is made of a thermosetting resin for a semiconductor device using the first aspect. The substance is filled in the above gap and hardened. Photo-semiconductor According to a fifth aspect of the invention, the optical semiconductor device includes a light-emitting element having a wavelength of 350 to 410 nm at a predetermined position of a lead frame for an optical semiconductor device, and the lead frame for the optical semiconductor device includes a light-emitting element mounting region and is formed. The reflector is formed in a state in which at least a part of the reflector surrounds the periphery of the component mounting region, and the reflector is formed of a thermosetting resin composition for the optical semiconductor device according to the first aspect. to make.
本發明人等為了得到可取代以往的陶瓷材料且在近紫外線~紫外線之特定波長範圍中具有高的光反射率之光半導體裝置用熱硬化性樹脂組成物而反覆專心檢討。結果，查明在反射器材料方面，若在各種白色顏料當中選用氧化鋯，仍可達成所預期的目的。亦即，本發明人等反覆研究之後的結果，得到以下的知識見解：上述氧化鋯具備了在近紫外線~紫外線範圍之波長350~410nm中未顯現光吸收的特性。根據此知識見解反覆深入研究的結果，發現當僅使用氧化鋯來作為白色顏料時，對於特定波長範圍350~410nm的光可發揮高度的光反射率，並得以形成可取代以往的陶瓷材料之優異反射器形成材料。 In order to obtain a thermosetting resin composition for an optical semiconductor device which can replace a conventional ceramic material and has a high light reflectance in a specific wavelength range of near ultraviolet to ultraviolet light, the present inventors have repeatedly conducted intensive review. As a result, it was found that in terms of the material of the reflector, if zirconia is selected among various white pigments, the intended purpose can be attained. In other words, the inventors of the present invention have obtained the following knowledge and found that the zirconia has a characteristic that no light absorption occurs in the wavelength range of 350 to 410 nm in the near ultraviolet to ultraviolet range. Based on this knowledge, the results of in-depth research have found that when only zirconia is used as a white pigment, a high light reflectance can be exhibited for light having a specific wavelength range of 350 to 410 nm, and an excellent alternative to the conventional ceramic material can be formed. The reflector forms a material.
如所述，本發明之光半導體裝置用熱硬化性樹脂組成物，是作為具備波長350~410nm之發光元件之光半導體裝置的反射器形成材料來使用，並含有前述熱硬化性樹脂(A)與僅由氧化鋯形成之白色顏料(B)。因此，對上述特定波長範圍之光具有高的光反射率。所以，作為取代以往之 陶瓷材料的反射器形成材料是有用的，而藉由使用上述熱硬化性樹脂組成物可輕易形成各種反射器形狀，且可得到可靠性高之光半導體裝置。 As described above, the thermosetting resin composition for an optical semiconductor device of the present invention is used as a reflector forming material for an optical semiconductor device having a light-emitting element having a wavelength of 350 to 410 nm, and contains the thermosetting resin (A). White pigment (B) formed only of zirconia. Therefore, the light having the above specific wavelength range has a high light reflectance. So, as a substitute for the past A reflector forming material of a ceramic material is useful, and various reflector shapes can be easily formed by using the above thermosetting resin composition, and a highly reliable optical semiconductor device can be obtained.
此外，當使用無機質填充劑(C)時，可產生降低線膨脹係數之效果。 Further, when the inorganic filler (C) is used, an effect of lowering the coefficient of linear expansion can be produced.
1‧‧‧第1板部 1‧‧‧1st Board
2‧‧‧第2板部 2‧‧‧2nd Board
3‧‧‧光半導體元件 3‧‧‧Optical semiconductor components
4,11‧‧‧反射器 4,11‧‧‧ reflector
5‧‧‧凹部 5‧‧‧ recess
6‧‧‧密封樹脂層 6‧‧‧ sealing resin layer
7、8、12‧‧‧接合線 7, 8, 12‧‧ ‧ bonding wire
10‧‧‧金屬引線框 10‧‧‧Metal lead frame
圖1為示意性表示光半導體裝置之構成的截面圖。 Fig. 1 is a cross-sectional view schematically showing the configuration of an optical semiconductor device.
圖2為示意性表示光半導體裝置之其他構成的俯視圖。 FIG. 2 is a plan view schematically showing another configuration of the optical semiconductor device.
圖3為示意性表示上述光半導體裝置其他構成之俯視圖的X-X'箭頭指向截面圖。 3 is a cross-sectional view taken along the line XX' of the plan view showing another configuration of the optical semiconductor device.
本發明之光半導體裝置用熱硬化性樹脂組成物(以下，也稱為「熱硬化性樹脂組成物」)，是作為例如後述圖1所示光半導體裝置或圖2及圖3所示光半導體裝置的反射器形成材料來使用，且是使用熱硬化性樹脂(A成分)與特定之白色顏料(B成分)而得到者，通常是作成液狀、片狀、或粉末狀，或是將該粉末打錠成錠狀以供反射器形成材料使用。並且，本發明之熱硬化性樹脂組成物是以光半導體裝置中的反射器形成材料作為使用對象，且該光半導體裝置具備可發出近紫外線~紫外線範圍之波長350~410nm之光的發光元件。 The thermosetting resin composition for an optical semiconductor device of the present invention (hereinafter also referred to as "thermosetting resin composition") is, for example, an optical semiconductor device shown in FIG. 1 described later or an optical semiconductor shown in FIGS. 2 and 3. The reflector of the device is used as a material, and is obtained by using a thermosetting resin (component A) and a specific white pigment (component B), usually in the form of a liquid, a sheet, or a powder, or The powder is ingots in the form of a pellet for use in a reflector forming material. Further, the thermosetting resin composition of the present invention is used as a reflector forming material in an optical semiconductor device, and the optical semiconductor device includes a light-emitting element capable of emitting light having a wavelength of 350 to 410 nm in a range of near ultraviolet to ultraviolet.
<A：熱硬化性樹脂> <A: Thermosetting resin>
上述熱硬化性樹脂(A成分)可列舉出例如，環氧樹脂、矽氧樹脂等。該等熱硬化樹脂可單獨或合併使用。 The thermosetting resin (component A) may, for example, be an epoxy resin or a silicone resin. These thermosetting resins may be used singly or in combination.
上述環氧樹脂可列舉出例如，雙酚A型環氧樹脂、雙酚F型環氧樹脂、雙酚S型環氧樹脂、酚系酚醛清漆型環氧樹脂及甲酚酚醛清漆型環氧樹脂等之酚醛清漆型環氧樹脂，異三聚氰酸單環氧丙酯、異三聚氰酸二環氧丙酯、異三聚氰酸三環氧丙酯、海因環氧樹脂等之含氮環環氧樹脂，氫化雙酚A型環氧樹脂、氫化雙酚F型環氧樹脂、脂肪族環氧樹脂、矽氧變性環氧樹脂、環氧丙基醚型環氧樹脂、烷基取代雙酚等之二環氧丙基醚、藉由二胺苯甲烷及異三聚氰酸等之聚胺與表氯醇反應製得之環氧丙基胺型環氧樹脂、藉由過乙酸等之過酸氧化烯烴鍵而製得之線狀脂肪族及脂環式環氧樹脂、低吸水率硬化體型之主流聯苯型環氧樹脂、二環環型環氧樹脂、萘型環氧樹脂等。該等環氧樹脂可單獨或合併2種以上使用。這些環氧樹脂之中，從具優異透明性以及耐變色性方面來看，宜單獨或合併使用脂環式環氧樹脂，或具有異三聚氰酸三環氧丙酯等之異三聚氰酸酯環構造的環氧樹脂。由相同的理由來看，苯二甲酸、四氫鄰苯二甲酸、六氫鄰苯二甲酸、甲基四氫鄰苯二甲酸、降冰片烯二酸、甲基降冰片烯二酸等之二羧酸的二環氧丙基酯也是合適的。又，也可舉具有芳香環氫化之脂環式構造的核氫化三苯六甲酸、核氫化焦蜜石酸等環氧丙基酯等為例。 Examples of the epoxy resin include bisphenol A epoxy resin, bisphenol F epoxy resin, bisphenol S epoxy resin, phenol novolak epoxy resin, and cresol novolak epoxy resin. Such as phenolic varnish type epoxy resin, iso-glycidyl monoglycidyl acrylate, iso-glycidyl diglycidyl ester, iso-glycidyl methacrylate, hydantoin epoxy resin, etc. Nitrogen ring epoxy resin, hydrogenated bisphenol A epoxy resin, hydrogenated bisphenol F epoxy resin, aliphatic epoxy resin, epoxy modified epoxy resin, epoxy propyl ether epoxy resin, alkyl substitution a diglycidyl ether such as bisphenol, a epoxypropylamine type epoxy resin obtained by reacting a polyamine such as diaminophenylmethane or isomeric cyanuric acid with epichlorohydrin, by peracetic acid or the like Linear aliphatic and alicyclic epoxy resins obtained by acid oxidation of olefin bonds, mainstream biphenyl type epoxy resins having low water absorption and hardening type, bicyclic ring type epoxy resins, naphthalene type epoxy resins, etc. . These epoxy resins may be used alone or in combination of two or more. Among these epoxy resins, from the viewpoint of excellent transparency and discoloration resistance, it is preferred to use an alicyclic epoxy resin alone or in combination, or a isomeric cyanide having a triglycidyl isocyanurate or the like. An epoxy resin constructed of an acid ester ring. For the same reason, phthalic acid, tetrahydrophthalic acid, hexahydrophthalic acid, methyltetrahydrophthalic acid, norbornene diacid, methylnorbornene diacid, etc. Di-epoxypropyl esters of carboxylic acids are also suitable. Further, examples thereof include nuclear hydrogenated triphenyl hexacarboxylic acid having an alicyclic structure of an aromatic ring hydrogenation, and a glycidyl ester such as nuclear hydrogenated pyrophoric acid.
上述環氧樹脂在常溫下可以是固形或液狀，但 是，一般而言，使用之環氧樹脂的平均環氧當量宜為90~1000，又，為固形時，從處理性之方便性的觀點來看，軟化點宜為50~160℃。亦即，環氧當量過小時，有時熱硬化性樹脂組成物硬化物會脆化。又，環氧當量過大時，可看到熱硬化性樹脂組成物硬化物之玻璃轉移溫度(Tg)降低的傾向。 The above epoxy resin may be solid or liquid at normal temperature, but In general, the epoxy resin used has an average epoxy equivalent of from 90 to 1,000. Further, when it is in a solid form, the softening point is preferably from 50 to 160 ° C from the viewpoint of handling convenience. That is, when the epoxy equivalent is too small, the cured product of the thermosetting resin composition may be embrittled. Further, when the epoxy equivalent is too large, the glass transition temperature (Tg) of the cured product of the thermosetting resin composition tends to decrease.
使用上述環氧樹脂作為熱硬化性樹脂(A成分)時，通常，可使用硬化劑。上述硬化劑可舉酐系硬化劑、異三聚氰酸衍生物系硬化劑等為例。該等硬化劑可單獨或合併2種以上使用。該等硬化劑中，從耐熱性及耐光性的觀點來看，宜使用酐系硬化劑。 When the above epoxy resin is used as the thermosetting resin (component A), a curing agent can be usually used. The curing agent may, for example, be an anhydride-based curing agent or a different isocyanuric acid derivative-based curing agent. These hardeners can be used individually or in combination of 2 or more types. Among these hardeners, an anhydride-based curing agent is preferably used from the viewpoint of heat resistance and light resistance.
上述酐系硬化劑可列舉出例如，苯二甲酐、馬來酐、琥珀酐、三苯六甲酐、焦蜜石酐、萘-1,4,5,8-四羧酸二酐及其核氫化物、六氫鄰苯二甲酐、3-甲基六氫鄰苯二甲酐、4-甲基六氫鄰苯二甲酐、四氫鄰苯二甲酐、3-甲基四氫鄰苯二甲酐、4-甲基四氫鄰苯二甲酐、甲基降冰片烯二酐、環己烷-1,2,3-三羧酸-2,3-酐及其位置異構物、環己烷-1,2,3,4-四羧酸-3,4-酐及其位置異構物、降冰片烯二酐、戊二酐、二甲基戊二酐、二乙基戊二酐、甲基六氫鄰苯二甲酐、甲基四氫鄰苯二甲酐等。該等酐系硬化劑可單獨或合併2種以上使用。又，具有該等酐作為飽和脂肪鏈骨架、不飽和脂肪鏈骨架，或矽氧骨架之端基或側鏈之寡聚物，亦可單獨或合併2種以上，以及與上述酐合併而使用。在這些酐系硬化劑中，宜使用苯二甲酐、六氫鄰苯二甲酐、3-甲 基六氫鄰苯二甲酐、4-甲基六氫鄰苯二甲酐、四氫鄰苯二甲酐、3-甲基四氫鄰苯二甲酐、4-甲基四氫鄰苯二甲酐。此外，酐系硬化劑，宜使用無色或淡黃色的酐系硬化劑。又，也可以併用上述酐之水解物的羧酸。 Examples of the anhydride-based curing agent include phthalic anhydride, maleic anhydride, succinic anhydride, trimellitic anhydride, pyrogalic anhydride, naphthalene-1,4,5,8-tetracarboxylic dianhydride, and a core thereof. Hydride, hexahydrophthalic anhydride, 3-methylhexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, tetrahydrophthalic anhydride, 3-methyltetrahydroortho Phthalic anhydride, 4-methyltetrahydrophthalic anhydride, methylnorbornene dianhydride, cyclohexane-1,2,3-tricarboxylic acid-2,3-anhydride and its positional isomers , cyclohexane-1,2,3,4-tetracarboxylic acid-3,4-anhydride and its positional isomers, norbornene dianhydride, glutaric anhydride, dimethyl glutaric anhydride, diethyl pentane Dihydride, methylhexahydrophthalic anhydride, methyltetrahydrophthalic anhydride, and the like. These anhydride-based curing agents may be used singly or in combination of two or more. Further, an oligomer having such an anhydride as a saturated aliphatic chain skeleton, an unsaturated aliphatic chain skeleton, or an end group or a side chain of a fluorene skeleton may be used singly or in combination of two or more kinds thereof and in combination with the above-mentioned anhydride. Among these anhydride hardeners, it is preferred to use phthalic anhydride, hexahydrophthalic anhydride, 3-methyl Hexahydrophthalic anhydride, 4-methylhexahydrophthalic anhydride, tetrahydrophthalic anhydride, 3-methyltetrahydrophthalic anhydride, 4-methyltetrahydroortylene Meal anhydride. Further, as the anhydride-based curing agent, a colorless or pale yellow anhydride-based curing agent is preferably used. Further, a carboxylic acid of the hydrolyzate of the above anhydride may be used in combination.
又，上述異三聚氰酸衍生物系硬化劑可列舉出例如，1,3,5-三(1-羧甲基)異三聚氰酸酯、1,3,5-三(2-羧乙基)異三聚氰酸酯、1,3,5-三(3-羧丙基)異三聚氰酸酯、1,3-二(2-羧乙基)異三聚氰酸酯等。該等異三聚氰酸衍生物系硬化劑可單獨或合併2種以上使用。此外，異三聚氰酸衍生物系硬化劑宜使用無色或淡黃色的硬化劑。 Further, examples of the above-mentioned isocyanuric acid derivative-based curing agent include 1,3,5-tris(1-carboxymethyl)isocyanate and 1,3,5-tris(2-carboxyl). Ethyl)isomeric cyanurate, 1,3,5-tris(3-carboxypropyl)isocyanate, 1,3-bis(2-carboxyethyl)isocyanate, etc. . These isomeric cyanuric acid derivative-based curing agents may be used singly or in combination of two or more kinds. Further, as the hardening agent for the isocyanuric acid derivative, a colorless or pale yellow hardener is preferably used.
在此，上述環氧系樹脂與上述硬化劑之摻混比例宜設定成，相對於環氧系樹脂中的環氧基1當量，使硬化劑中可與環氧基反應的活性基(酐基或羧基)為0.3~1.3當量，更佳是0.5~1.1當量。亦即，這是因為活性基過少時，會看到熱硬化性樹脂組成物的硬化速度變慢，且其硬化物之玻璃轉移溫度(Tg)降低的傾向，當活性基過多時可看到耐濕性降低的傾向。 Here, the blending ratio of the epoxy resin and the curing agent is preferably set to an active group capable of reacting with an epoxy group in the curing agent with respect to 1 equivalent of the epoxy group in the epoxy resin. Or carboxyl group) is from 0.3 to 1.3 equivalents, more preferably from 0.5 to 1.1 equivalents. In other words, when the number of active groups is too small, the curing rate of the thermosetting resin composition is slow, and the glass transition temperature (Tg) of the cured product tends to decrease. When the number of active groups is too large, resistance is observed. The tendency to reduce wetness.
又，因應其目的以及用途，可將前面所提到的上述酐系硬化劑以及異三聚氰酸衍生物系硬化劑以外的其他環氧樹脂系硬化劑，例如，酚系硬化劑、胺系硬化劑、藉醇部分酯化上述酐系硬化劑等之硬化劑單獨或合併2種以上使用。再者，使用這些硬化劑時，其摻混比例亦可以上述環氧樹脂與硬化劑之摻混比例(當量比)為準。 In addition, the above-mentioned anhydride-based curing agent and other epoxy resin-based curing agent other than the isocyanuric acid derivative-based curing agent may be used, for example, a phenol-based curing agent or an amine system. The curing agent or the curing agent such as the above-mentioned anhydride-based curing agent, which is partially esterified with an alcohol, may be used singly or in combination of two or more kinds. Further, when these hardeners are used, the blending ratio thereof may be based on the blending ratio (equivalent ratio) of the epoxy resin and the hardener.
接下來，針對使用上述矽氧樹脂作為上述熱硬化 性樹脂(A成分)之情形作說明。上述矽氧樹脂，至少含有觸媒，具體來說，含有觸媒及矽氧樹脂。上述觸媒是例如促進矽氧樹脂之反應而使矽氧樹脂硬化的硬化觸媒，較理想的是促進後述之矽氧樹脂的矽氫化反應以藉由氫矽加成使矽氧樹脂硬化的矽氫化觸媒。並且，上述觸媒含有過渡金屬，且上述過渡金屬可舉例如白金、鈀、銠等之白金屬元素，且較佳為白金。具體而言，在觸媒含有白金時，作為觸媒可列舉出例如，白金黑、氯化白金、氯化白金酸等之無機白金；例如，白金-烯烴錯合物、白金-羰基錯合物、白金-乙醯乙酸等之白金錯合物等，且較理想的是白金錯化合物。更具體來說，作為白金錯合物，可列舉出例如，白金-乙烯矽氧烷錯合物、白金-四甲基二乙烯二矽氧烷錯合物、白金-羰基環乙烯甲基矽氧烷錯合物、白金-二乙烯基四甲基二矽氧烷錯合物、白金-環乙烯甲基矽氧烷錯合物、白金-辛醛/辛醇錯合物等。再者，上述觸媒具有與後述之矽氧樹脂區別地摻混之態樣，或包含於矽氧樹脂中作為構成矽氧樹脂之成分的態樣。 Next, the above-mentioned silicone resin is used as the above-mentioned thermosetting The case of the resin (component A) is explained. The above-mentioned epoxy resin contains at least a catalyst, and specifically contains a catalyst and a silicone resin. The catalyst is, for example, a curing catalyst which promotes the reaction of the epoxy resin to harden the epoxy resin, and is preferably a crucible which promotes the hydrogenation reaction of the neodymium resin described later to harden the epoxy resin by hydroquinone addition. Hydrogenation catalyst. Further, the catalyst contains a transition metal, and the transition metal may, for example, be a white metal element such as platinum, palladium or rhodium, and is preferably platinum. Specifically, when the catalyst contains platinum, examples of the catalyst include inorganic platinum such as platinum black, chlorinated platinum, and chloroplatinic acid; for example, platinum-olefin complex, platinum-carbonyl complex. A platinum complex such as platinum-acetic acid or the like, and preferably a platinum compound. More specifically, as the platinum complex, for example, platinum-vinyloxane complex, platinum-tetramethyldiethylenedioxane complex, platinum-carbonylcyclovinylmethyloxime An alkane complex, a platinum-divinyltetramethyldioxane complex, a platinum-cyclovinylmethyloxane complex, a platinum-octanal/octanol complex, and the like. Further, the above-mentioned catalyst has a state in which it is blended differently from the above-described oxime resin, or is contained in the oxime resin as a component constituting the oxime resin.
上述觸媒中之過渡金屬的含有比例(濃度)，相對矽氧樹脂整體，在質量基準下，宜為0.1~500ppm，較佳為0.15~100ppm，更佳為0.2~50ppm，特佳為0.3~10ppm。 The content ratio (concentration) of the transition metal in the catalyst is preferably 0.1 to 500 ppm, preferably 0.15 to 100 ppm, more preferably 0.2 to 50 ppm, and particularly preferably 0.3 to 50% by mass based on the mass of the epoxy resin. 10ppm.
上述矽氧樹脂是藉觸媒促進反應而硬化之硬化性矽氧樹脂，且可列舉出例如，1階硬化型矽氧樹脂、2階硬化型矽氧樹脂等之熱硬化性矽氧樹脂等。 The above-mentioned oxime resin is a curable oxime resin which is cured by a catalyst to promote the reaction, and examples thereof include a thermosetting oxime resin such as a first-order curable oxime resin and a second-order curable oxime resin.
上述2階硬化型矽氧樹脂具有2階段之反應機 構，且是在第1階反應中B階段化(半硬化)，在第2階反應中C階段化(完全硬化)之熱硬化性矽氧樹脂。再者，上述之B階段是熱硬化性矽氧樹脂在可溶於溶劑之A階段與完全硬化之C階段間的狀態，且是稍微進行硬化及凝膠化，且在溶劑中膨潤，但未完全溶解，並且藉加熱軟化但未熔融之狀態。 The above-mentioned second-order hardening type epoxy resin has a two-stage reaction machine It is a thermosetting oxime resin which is B-staged (semi-hardened) in the first-order reaction and C-staged (completely hardened) in the second-order reaction. Further, the above-mentioned B-stage is a state in which the thermosetting oxime resin is in a state in which the solvent is soluble in the A phase and the fully cured C phase, and is slightly hardened and gelled, and swelled in a solvent, but not It is completely dissolved and softened by heat but not melted.
上述1階硬化型矽氧樹脂具有1階段之反應機構，且是在第1階反應中完全硬化的熱硬化性矽氧樹脂。作為上述1階硬化型矽氧樹脂，可舉日本專利特開2012-124428號公報所揭示的加成反應硬化型聚有機聚矽氧烷為例。具體而言，加成反應硬化型聚有機聚矽氧烷，含有例如，含乙烯系不飽和烴基矽化合物以及含矽氫基矽化合物。 The first-stage hardening type oxime resin has a one-stage reaction mechanism and is a thermosetting oxime resin which is completely cured in the first-order reaction. The addition-curing type polyorganopolyoxyalkylene disclosed in Japanese Laid-Open Patent Publication No. 2012-124428 is exemplified as the first-order curing type oxime resin. Specifically, the addition reaction-curable polyorganopolysiloxane contains, for example, an ethylenically unsaturated hydrocarbon group-containing compound and a ruthenium-containing ruthenium-containing compound.
作為上述含乙烯系不飽和烴基矽化合物可列舉出例如，在分子內有2個以上之乙烯基之含乙烯基聚有機矽氧烷，且較理想的是兩末端乙烯聚二甲基矽氧烷。 The vinyl-containing unsaturated hydrocarbon-based ruthenium compound may, for example, be a vinyl-containing polyorganosiloxane having two or more vinyl groups in the molecule, and more preferably a two-terminal ethylene polydimethyl siloxane. .
作為上述含矽氫基矽化合物可列舉出例如，在分子內有2個以上之矽氫基之含矽氫基聚有機矽氧烷，且較理想的是兩末端矽氫聚二甲基矽氧烷、兩末端三甲基矽基封鎖甲基氫矽氧烷-二甲基矽氧烷共聚物等。 Examples of the ruthenium-containing ruthenium-containing ruthenium compound include a ruthenium-hydrogen group-containing polyorganosiloxane having two or more ruthenium hydrogen groups in the molecule, and more preferably two-terminal oxime hydrogen polydimethyl oxime The alkane and the terminal trimethylsulfonyl group block the methylhydroquinone-dimethyloxane copolymer and the like.
作為上述2階硬化型矽氧樹脂可舉例如具有縮合反應與加成反應之2反應系之縮合反應‧加成反應硬化型矽氧樹脂等。這種縮合反應‧加成反應硬化型矽氧樹脂含有觸媒，且可列舉以下諸樹脂為例：如，第1縮合反應‧加成 反應硬化型矽氧樹脂，其含有矽烷醇兩末端聚矽氧烷、含烯基三烷氧基矽烷、有機氫聚矽氧烷、縮合觸媒及矽氫化觸媒；例如，第2縮合反應‧加成反應硬化型矽氧樹脂，其含有矽烷醇基兩末端聚矽氧烷、含乙烯系不飽和烴基矽化合物、含乙烯系不飽和烴基矽化合物、有機氫聚矽氧烷、縮合觸媒及矽氫化觸媒；例如，第3縮合反應‧加成反應硬化型矽氧樹脂，其含有兩末端矽烷醇型聚矽氧油、含烯基二烷氧烷基矽烷、有機氫聚矽氧烷、縮合觸媒及矽氫化觸媒；例如，第4縮合反應‧加成反應硬化型矽氧樹脂，其含有在1分子中具有至少2個烯基矽基之有機聚矽氧烷、在1分子中具有至少2個矽氫基之有機聚矽氧烷、矽氫化觸媒及硬化延遲劑；例如，第5縮合反應‧加成反應硬化型矽氧樹脂，其含有在1分子中合併具有至少2個乙烯系不飽和烴基與至少2個矽氫基之第1有機聚矽氧烷、不含乙烯系不飽和烴基且在1分子中具有至少2個矽氫基之第2有機聚矽氧烷、矽氫化觸媒及矽氫化抑制劑；例如，第6縮合反應‧加成反應硬化型矽氧樹脂，其含有在1分子中合併具有至少2個乙烯系不飽和烴基與至少2個矽烷醇基之第1有機聚矽氧烷、不含乙烯系不飽和烴基且在1分子中具有至少2個矽氫基之第2有機聚矽氧烷、矽氫化抑制劑及矽氫化觸媒； 例如，第7縮合反應‧加成反應硬化型矽氧樹脂，其含有矽化合物以及硼化合物或鋁化合物；例如，第8縮合反應‧加成反應硬化型矽氧樹脂，其含有聚鋁矽氧烷以及矽烷耦合劑。 The second-stage hardening type oxime resin may, for example, be a condensation reaction of a reaction system having a condensation reaction and an addition reaction, or an addition reaction-type oxime resin. This condensation reaction ‧ addition reaction hardening type oxiran resin contains a catalyst, and the following resins are exemplified: for example, the first condensation reaction ‧addition a reaction-curing type anthracene resin comprising a decyl alcohol two-terminal polyoxyalkylene oxide, an alkenyl group-containing trialkoxy decane, an organic hydrogen polyoxyalkylene oxide, a condensation catalyst, and a ruthenium hydrogenation catalyst; for example, a second condensation reaction An addition reaction-hardening type oxiran resin comprising a decyl alcohol-based two-terminal polyoxyalkylene oxide, an ethylenically unsaturated hydrocarbon-based ruthenium compound, an ethylenically unsaturated hydrocarbon-based ruthenium compound, an organohydrogenpolysiloxane, a condensation catalyst, and a hydrogenation catalyst; for example, a third condensation reaction ‧ addition reaction hardening type oxiran resin containing a terminal stanol type polyphthalic acid oil, an alkenyl dialkoxyalkyl decane, an organic hydrogen polyoxy siloxane, a condensation catalyst and a hydrazine hydrogenation catalyst; for example, a fourth condensation reaction ‧ an addition reaction hardening type oxiran resin containing an organopolysiloxane having at least two alkenyl fluorenyl groups in one molecule, in one molecule An organopolyoxyalkylene having at least 2 anthracene hydrogen groups, a hydrazine hydrogenation catalyst, and a hardening retarder; for example, a fifth condensation reaction ‧ addition reaction hardening type oxiran resin containing at least 2 combined in one molecule Ethylene-based unsaturated hydrocarbon group and at least two anthracene hydrogen groups a first organopolyoxane, a second organopolyoxane having at least two anthracene hydrogen groups in one molecule, and a hydrogenation catalyst and a hydrazine hydrogenation inhibitor; for example, the sixth Condensation reaction ‧ addition reaction hardening type oxirane containing a first organopolyoxane having at least two ethylenically unsaturated hydrocarbon groups and at least two stanol groups in one molecule, and no ethylenic unsaturation a second organopolyoxane having a hydrocarbon group and having at least two anthracene hydrogen groups in one molecule, a hydrazine hydrogenation inhibitor, and a hydrazine hydrogenation catalyst; For example, a seventh condensation reaction ‧ an addition reaction hardening type oxiran resin containing a ruthenium compound and a boron compound or an aluminum compound; for example, an eighth condensation reaction ‧ addition reaction hardening type oxiran resin containing polyaluminoxane And a decane coupling agent.
這些縮合反應‧加成反應硬化型矽氧樹脂可單獨或合併2種以上使用。 These condensation reaction ‧ addition reaction hardening type epoxy resins may be used singly or in combination of two or more.
作為上述縮合反應‧加成反應硬化型矽氧樹脂，較理想的可舉上述第2縮合反應‧加成反應硬化型矽氧樹脂為例，具體而言，詳細記載於日本專利特開2010-265436號公報等上，例如，含有矽烷醇基兩末端聚二甲基矽氧烷、乙烯三甲氧基矽烷、(3-環氧丙氧基丙基)三甲氧基矽烷、二甲聚矽氧烷-co-甲基氫聚矽氧烷、羥化四甲基銨以及白金-羰基錯合物。具體而言，為調製上述第2縮合反應‧加成反應硬化型矽氧樹脂時，可藉由例如，首先，一次添加縮合原料之含乙烯系不飽和烴基矽化合物及含乙烯系不飽和烴基矽化合物與縮合觸媒，接著，添加加成原料之有機氫聚矽氧烷，然後，添加矽氫化觸媒(加成觸媒)來調製。 The condensation reaction ‧ addition reaction-curing type oxime resin is preferably exemplified by the second condensation reaction ‧ addition reaction-curable oxime resin, and specifically described in Japanese Patent Laid-Open No. 2010-265436 The commemorative article or the like, for example, contains a decyl alcohol group at both ends of polydimethyl siloxane, ethylene trimethoxy decane, (3-glycidoxypropyl) trimethoxy decane, dimethyl polyoxy siloxane - Co-methylhydrogenpolysiloxane, hydroxylated tetramethylammonium, and platinum-carbonyl complex. Specifically, when the second condensation reaction ‧ addition reaction-curing type oxime resin is prepared, for example, the ethylenically unsaturated hydrocarbon group-containing compound and the ethylenically unsaturated hydrocarbon group containing a condensation raw material may be added at a time. The compound and the condensation catalyst are then added to the organic hydrogen polyoxyalkylene of the addition starting material, followed by addition of a ruthenium hydrogenation catalyst (addition catalyst).
<B：特定之白色顏料> <B: Specific white pigment>
本發明中的特徵為白色顏料僅由氧化鋯(ZrO2)所構成。亦即，本發明中，其特徵在於，白色顏料，實質上僅由氧化鋯所構成，不似以往使用在有機系反射器材料中所使用的氧化鈦與氧化鋅等其他白色顏料。作為上述氧化鋯，從流動性等之觀點來看，較理想的是使用平均粒徑為0.01~50μm的氧化鋯，特別理想的是使用0.1~20μm的。再 者，上述平均粒徑可由例如雷射繞射散射式粒度分布計來測量。 The feature in the present invention is that the white pigment consists solely of zirconia (ZrO 2 ). That is, in the present invention, the white pigment is substantially composed only of zirconia, and other white pigments such as titanium oxide and zinc oxide used in the organic reflector material are not used. As the zirconia, it is preferable to use zirconia having an average particle diameter of 0.01 to 50 μm from the viewpoint of fluidity and the like, and it is particularly preferable to use 0.1 to 20 μm. Further, the above average particle diameter can be measured by, for example, a laser diffraction scattering type particle size distribution meter.
上述氧化鋯(B成分)之含有比率，相對於熱硬化性樹脂組成物整體，宜為2~30體積%，較佳為5~30體積%。亦即，B成分之含有比率過小時，會看到難以獲得充分之光反射性的傾向。B成分之含有比率過大時，會看到因為顯著增黏而可能在有關藉混煉等進行的熱硬化性樹脂組成物的製作上產生困難。 The content ratio of the zirconia (component B) is preferably 2 to 30% by volume, and preferably 5 to 30% by volume based on the entire thermosetting resin composition. In other words, when the content ratio of the component B is too small, it is difficult to obtain sufficient light reflectivity. When the content ratio of the component B is too large, it may be difficult to produce a thermosetting resin composition by kneading or the like due to remarkably thickening.
<C：無機質填充劑> <C: Inorganic filler>
此外，在本發明中，可與上述A及B成分一起使用無機質填充劑(C成分)。作為上述無機質填充劑(C成分)，可列舉出例如，石英玻璃粉末、滑石、熔融二氧化矽粉末或結晶性二氧化矽粉末等之二氧化矽粉末、氧化鋁粉末、氮化鋁粉末、氮化矽粉末等。其中，從線膨脹係數降低等的觀點來看，尤以使用熔融二氧化矽粉末為宜，特別地，從高填充性及高流動性的觀點來看，宜使用熔融球狀二氧化矽粉末。再者，無機質填充劑(C成分)是在上述特定之白色顏料(B成分)以外。有關上述無機質填充劑(C成分)之粒徑及其分布，宜考慮使上述特定白色顏料(B成分)之粒徑以及其分布之組合，在藉由轉移成形等成形熱硬化性樹脂組成物時之毛邊等減到最少。具體而言，無機質填充劑(C成分)之平均粒徑宜為5~100μm，較佳是10~80μm。再者，與前述相同地，上述平均粒徑可使用例如雷射繞射散射式粒度分布計來測量。 Further, in the present invention, an inorganic filler (component C) can be used together with the above components A and B. Examples of the inorganic filler (component C) include ceria powder such as quartz glass powder, talc, molten cerium oxide powder or crystalline cerium oxide powder, alumina powder, aluminum nitride powder, and nitrogen. Pupation powder and the like. Among them, from the viewpoint of a reduction in the coefficient of linear expansion, etc., it is preferable to use molten cerium oxide powder, and in particular, from the viewpoint of high filling property and high fluidity, it is preferable to use molten spherical cerium oxide powder. Further, the inorganic filler (component C) is other than the specific white pigment (component B) described above. In the particle size and the distribution of the inorganic filler (component C), it is preferable to use a combination of the particle diameter and the distribution of the specific white pigment (component B) to form a thermosetting resin composition by transfer molding or the like. The burrs and the like are minimized. Specifically, the inorganic filler (component C) preferably has an average particle diameter of 5 to 100 μm, preferably 10 to 80 μm. Further, as described above, the above average particle diameter can be measured using, for example, a laser diffraction scattering type particle size distribution meter.
並且，在上述無機質填充劑(C成分)之含有比率中，上述特定白色顏料(B成分)與無機質填充劑(C成分)之合計的含有比率宜設定在熱硬化性樹脂組成物整體之75~90體積%。較佳是75~85體積%。亦即，上述合計的含有比率過小時，會看到產生在成形時發生翹曲等問題的傾向。又，合計的含有比率過大時，會看到在將摻混成分混煉時，對混煉機施加莫大的負載，且變成無法混煉的傾向，結果，會看到製作成形材料之熱硬化性樹脂組成物變困難之傾向。 In addition, in the content ratio of the inorganic filler (component C), the total content ratio of the specific white pigment (component B) and the inorganic filler (component C) is preferably set to 75 of the entire thermosetting resin composition. 90% by volume. It is preferably 75 to 85% by volume. In other words, when the total content ratio is too small, there is a tendency that problems such as warpage occur during molding. In addition, when the total content ratio is too large, it is seen that when the blended component is kneaded, a large load is applied to the kneader, and the kneading tends to be impossible, and as a result, the thermosetting property of the molded material is observed. The resin composition tends to be difficult.
此外，合併使用上述特定白色顏料(B成分)與無機質填充劑(C成分)時之兩者的混合比例，從初期光反射率的觀點來看，以體積比計，(B成分)/(C成分)=0.028~1.0是較理想的，特別理想的是0.033~0.50。亦即，B成分與C成分之混合比例在上述範圍外，且體積比過小時，會看到環氧樹脂組成物之初期光反射率降低的傾向，體積比過大時，會看到環氧樹脂組成物之熔融黏度上升而使混煉變困難之傾向。 In addition, the mixing ratio of the specific white pigment (component B) and the inorganic filler (component C) is used in combination, from the viewpoint of the initial light reflectance, (B component) / (C) The composition) = 0.028 to 1.0 is preferable, and particularly preferably 0.033 to 0.50. That is, when the mixing ratio of the component B and the component C is outside the above range, and the volume ratio is too small, the initial light reflectance of the epoxy resin composition tends to decrease, and when the volume ratio is too large, the epoxy resin is observed. The melt viscosity of the composition rises and the kneading tends to be difficult.
<其他添加劑> <Other additives>
並且，本發明之熱硬化性樹脂組成物，除了上述A及B成分，以及C成分以外，可視需要摻混硬化促進劑、脫模劑、矽烷化合物。此外，還可適宜地摻混變性劑(可塑劑)、抗氧化劑、阻燃劑、消泡劑、均染劑(leveling agent)、紫外線吸收劑等之各種添加劑。 Further, in addition to the above-mentioned components A and B and the component C, the thermosetting resin composition of the present invention may optionally contain a curing accelerator, a releasing agent, and a decane compound. Further, various additives such as a denaturant (plasticizer), an antioxidant, a flame retardant, an antifoaming agent, a leveling agent, an ultraviolet absorber, and the like may be blended as appropriate.
作為上述硬化促進劑，可列舉出例如，1,8-二氮 二環[5.4.0]十一烯-7、三伸乙二胺、三-2,4,6-二甲胺甲苯酚、N,N-二甲苄胺、N,N-二甲胺苯、N,N-二甲胺環己烷等之3級胺類、2-乙基-4-甲基咪唑、2-甲基咪唑等之咪唑類、三苯膦、四苯鏻四氟硼酸鹽、四苯鏻四苯硼酸鹽、四-n-丁鏻溴化物、四苯鏻溴化物、甲基三丁鏻二甲磷酸鹽、四苯鏻-o,o-二乙磷二硫代酸鹽、四-n-丁鏻-o,o-二乙磷二硫代酸鹽等之磷化合物、1,8-二氮二環[5.4.0]十一烯-7、三伸乙二銨辛羧酸鹽等之4級銨鹽、有機金屬鹽類、及其等的衍生物等。這些硬化促進劑可以單獨或合併2種以上使用。這些硬化促進劑之中，宜使用3級胺類、咪唑類、磷化合物。其中，為了得到著色度少，透明且強韌之硬化物，使用磷化合物是特別理想的。 The hardening accelerator may, for example, be 1,8-diaza Bicyclo [5.4.0] undecene-7, triamethylenediamine, tris-2,4,6-dimethylaminophenol, N,N-dimethylbenzylamine, N,N-dimethylamine benzene a third-grade amine such as N,N-dimethylamine cyclohexane, an imidazole such as 2-ethyl-4-methylimidazole or 2-methylimidazole, triphenylphosphine or tetraphenylphosphonium tetrafluoroborate , tetraphenylphosphonium tetraphenylborate, tetra-n-butane bromide, tetraphenylphosphonium bromide, methyltributylphosphonium phosphate, tetraphenylphosphonium-o,o-diethylphosphoric dithioate , a phosphorus compound such as tetra-n-butyl-o-o-diethylphosphoric dithioate, 1,8-diazabicyclo [5.4.0]undecene-7, triamethylene succinate a 4-grade ammonium salt such as a carboxylate, an organic metal salt, or the like, and the like. These hardening accelerators can be used individually or in combination of 2 or more types. Among these hardening accelerators, tertiary amines, imidazoles, and phosphorus compounds are preferably used. Among them, in order to obtain a cured product which is small in transparency and transparent and strong, it is particularly preferable to use a phosphorus compound.
上述硬化促進劑之含量，相對於上述特定之熱硬化性樹脂(A成分)，宜設定在0.001~8.0重量%，較佳為0.01~5重量%。亦即，這是因為硬化促進劑之含量過少時，有時無法得到充分的硬化促進效果，且硬化促進劑之含量過多時，可看到所製得之硬化物產生變色之傾向。 The content of the above-mentioned curing accelerator is preferably 0.001 to 8.0% by weight, preferably 0.01 to 5% by weight, based on the specific thermosetting resin (component A). That is, when the content of the hardening accelerator is too small, a sufficient curing acceleration effect may not be obtained, and when the content of the curing accelerator is too large, the cured product obtained tends to be discolored.
作為上述脫模劑，可使用各種脫模劑，其中又以使用具有醚鍵之脫模劑為佳，並可舉例如具備下述通式(1)所示之結構式的脫模劑。 As the above-mentioned release agent, various release agents can be used. Among them, a release agent having an ether bond is preferably used, and for example, a release agent having a structural formula represented by the following formula (1) can be used.
CH3‧(CH3)k‧CH2O(CHRm‧CHRn‧O)x‧H…(1) CH 3 ‧(CH 3 )k‧CH 2 O(CHRm‧CHRn‧O)x‧H...(1)
[式(1)中，Rm,Rn為氫原子或一價的烷基，且兩者可以互相相同亦可不同。又，k為1~100的正數，x為1~100的正 數。] [In the formula (1), Rm and Rn are a hydrogen atom or a monovalent alkyl group, and the two may be the same or different from each other. Also, k is a positive number from 1 to 100, and x is a positive one from 1 to 100. number. ]
在上述式(1)中，Rm,Rn為氫原子或一價的烷基，較佳地，k為10~50的正數，x為3~30的正數。更佳地，Rm及Rn為氫原子，k為28~48的正數，x為5~20的正數。亦即，重覆數k的值過小時，脫模性降低，且重覆數x的值過小時，分散性降低，因此可看到形成無法得到安定之強度與脫模性的傾向。另一方面，這是因為重覆數k的值過大時，可看到熔點變高，因此混煉變困難，且在熱硬化性樹脂組成物之製造步驟中產生困難的傾向，重覆數x的值過大時，則可看到脫模性降低的傾向。 In the above formula (1), Rm and Rn are a hydrogen atom or a monovalent alkyl group. Preferably, k is a positive number of 10 to 50, and x is a positive number of 3 to 30. More preferably, Rm and Rn are hydrogen atoms, k is a positive number from 28 to 48, and x is a positive number from 5 to 20. In other words, when the value of the number of repetitions k is too small, the mold release property is lowered, and the value of the number of repetitions x is too small, and the dispersibility is lowered. Therefore, the formation of strength and mold release property which cannot be stabilized can be observed. On the other hand, when the value of the number of repetitions k is too large, the melting point becomes high, so that kneading becomes difficult, and it tends to be difficult in the production step of the thermosetting resin composition, and the number of repetitions x When the value is too large, the tendency of the mold release property to be lowered is observed.
上述脫模劑之含量宜設定在熱硬化性樹脂組成物整體之0.001~3重量%的範圍內，較佳是設定在0.01~1重量%的範圍內。亦即，這是因為脫模劑之含量過少，或過多時，可看到造成硬化體之強度不足，或引起脫模性降低的傾向。 The content of the release agent is preferably set in the range of 0.001 to 3% by weight based on the entire thermosetting resin composition, and is preferably in the range of 0.01 to 1% by weight. That is, this is because when the content of the releasing agent is too small or too large, the strength of the hardened body is insufficient, or the mold release property tends to be lowered.
作為上述矽烷化合物，可舉矽烷耦合劑及矽烷為例。作為上述矽烷耦合劑，可列舉出例如，3-環氧丙氧基丙基甲基二甲氧矽烷、3-環氧丙氧基丙基三甲氧矽烷、3-環氧丙氧基丙基甲基二乙氧矽烷、3-環氧丙氧基丙基甲基乙氧矽烷、2-(3,4-環氧環己基)乙基三甲氧矽烷、3-巰丙基甲基二甲氧矽烷、3-巰丙基三甲氧矽烷等。又，作為上述矽烷，可列舉出例如，甲基三甲氧矽烷、二甲基二甲氧矽烷、苯基三甲氧矽烷、甲基三乙氧矽烷、二甲基二乙氧矽烷、苯基三乙氧矽烷、己基三甲氧矽烷、己基三乙氧矽烷、 癸基三甲氧矽烷、三氟丙基三甲氧矽烷、六甲基二矽氮烷、含水解基之矽氧烷等。該等矽烷可單獨或合併2種以上使用。 The decane compound may be exemplified by a decane coupling agent and decane. Examples of the above decane coupling agent include 3-glycidoxypropylmethyldimethoxydecane, 3-glycidoxypropyltrimethoxydecane, and 3-epoxypropoxypropyl group. Diethoxy oxane, 3-glycidoxypropyl methyl ethoxy decane, 2-(3,4-epoxycyclohexyl)ethyltrimethoxy decane, 3-mercaptopropylmethyldimethoxy decane , 3-mercaptopropyltrimethoxydecane, and the like. Further, examples of the decane include methyltrimethoxy decane, dimethyl dimethoxy decane, phenyl trimethoxy decane, methyl triethoxy decane, dimethyl diethoxy decane, and phenyl triethyl hydride. Oxy decane, hexyl trimethoxy decane, hexyl triethoxy decane, Mercapto trimethoxy decane, trifluoropropyltrimethoxy decane, hexamethyldioxane, a hydrolyzed group containing a hydrocarbyl group, and the like. These decanes may be used singly or in combination of two or more.
作為上述變性劑(可塑劑)，可舉乙二醇類、矽氧類、醇類等為例。 Examples of the above-mentioned denaturing agent (plasticizer) include ethylene glycols, oximes, alcohols, and the like.
作為上述抗氧化劑，可舉酚系化合物、胺系化合物、有機硫系化合物、磷系化合物等為例。 Examples of the antioxidant include a phenol compound, an amine compound, an organic sulfur compound, and a phosphorus compound.
作為上述阻燃劑，可列舉出例如，氫氧化鎂等之金屬氫氧化物、溴系阻燃劑、氮系阻燃劑、磷系阻燃劑等，亦可進一步使用三氧化二銻等阻燃助劑。 The flame retardant may, for example, be a metal hydroxide such as magnesium hydroxide, a bromine-based flame retardant, a nitrogen-based flame retardant or a phosphorus-based flame retardant, or may be further used such as antimony trioxide or the like. Fuel additives.
作為上述消泡劑，可舉矽氧系等習知的脫泡劑為例。 As the antifoaming agent, a conventional defoaming agent such as a ruthenium oxygen system can be exemplified.
<熱硬化性樹脂組成物> <Thermosetting resin composition>
本發明之熱硬化性樹脂組成物可用例如，如下所述的方式製造。亦即，可適當摻混上述A~C成分，硬化促進劑以及脫模劑，以及依需要使用之各種添加劑之後，使用混煉機等混煉以熔融混合，接下來，藉由將其冷卻且固化以進行粉碎，可以製造出粉末狀之熱硬化性樹脂組成物。 The thermosetting resin composition of the present invention can be produced, for example, in the following manner. In other words, the above-mentioned A to C component, a hardening accelerator, a releasing agent, and various additives as needed may be appropriately blended, and then kneaded by a kneader or the like to be melt-mixed, and then, by cooling and After curing to pulverize, a powdery thermosetting resin composition can be produced.
並且，作為上述所製得之熱硬化性樹脂組成物的硬化物，宜使其光反射率對波長350~410nm之光為在80%以上，更理想的是在83%以上。再者，上限通常為100%。上述光反射率是由例如，以下的方式來測量。亦即，藉由預定之硬化條件，例如，175℃×2分鐘的成形後，以175℃×3小時的後硬化製作厚度1mm之熱硬化性樹脂組成物的硬化 物，且藉由使用分光光度計(例如，日本分光公司製的分光光度計V-670)，以測量在室溫(25±10℃)下，上述範圍內之波長之上述硬化物的光反射率。 Further, the cured product of the thermosetting resin composition obtained as described above preferably has a light reflectance of 80% or more, more preferably 83% or more, of light having a wavelength of 350 to 410 nm. Furthermore, the upper limit is usually 100%. The above light reflectance is measured by, for example, the following method. That is, the hardening of the thermosetting resin composition having a thickness of 1 mm is formed by post-hardening at 175 ° C for 3 hours by predetermined hardening conditions, for example, after forming at 175 ° C for 2 minutes. And measuring the light reflection of the hardened substance at a wavelength within the above range at room temperature (25 ± 10 ° C) by using a spectrophotometer (for example, a spectrophotometer V-670 manufactured by JASCO Corporation) rate.
使用本發明之熱硬化性樹脂組成物作成的光半導體裝置是以例如以下的方式製造。亦即，將金屬引線框設置在轉移成形機之模具內，且使用上述熱硬化性樹脂組成物藉由轉移成形來形成反射器。依此進行，製作出以包圍光半導體元件裝載區域周圍之方式形成環狀反射器而成的光半導體裝置用之金屬引線框。接下來，將光半導體元件裝載在上述反射器內部之金屬引線框上的光半導體元件裝載區域，且使用接合線電性連接光半導體元件與金屬引線框。並且，使用矽氧樹脂等對包含上述光半導體元件之反射器內側區域進行樹脂密封，藉以形成密封樹脂層。如此進行，即可製作出例如圖1所示之立體狀(杯型)的光半導體裝置。該光半導體裝置是做成以下構成：在由第1板部1與第2板部2構成之金屬引線框的第2板部2上裝載光半導體元件3，且以包圍上述光半導體元件3周圍的方式，形成有由本發明之熱硬化性樹脂組成物構成之光反射用反射器4。並且，在上述金屬引線框及反射器4之內周面所形成之凹部5中，形成有密封光半導體元件3之具有透明性的密封樹脂層6。此密封樹脂層6上可依需要含有螢光體。在圖1中，7、8為電性連接形成於金屬引線框上之電極電路(圖未示)與光半導體元件3的接合線。 The optical semiconductor device formed using the thermosetting resin composition of the present invention is produced, for example, in the following manner. That is, the metal lead frame is placed in a mold of the transfer molding machine, and the reflector is formed by transfer molding using the above-described thermosetting resin composition. In this manner, a metal lead frame for an optical semiconductor device in which an annular reflector is formed so as to surround the periphery of the semiconductor device mounting region is formed. Next, the optical semiconductor element is mounted on the optical semiconductor element mounting region on the metal lead frame inside the reflector, and the optical semiconductor element and the metal lead frame are electrically connected using a bonding wire. Then, the inner region of the reflector including the optical semiconductor element is resin-sealed using a silicone resin or the like to form a sealing resin layer. In this way, a three-dimensional (cup type) optical semiconductor device as shown in Fig. 1 can be produced. In the optical semiconductor device, the optical semiconductor element 3 is mounted on the second plate portion 2 of the metal lead frame including the first plate portion 1 and the second plate portion 2, and surrounds the optical semiconductor element 3 In the embodiment, the light reflection reflector 4 composed of the thermosetting resin composition of the present invention is formed. Further, in the recessed portion 5 formed on the inner circumferential surface of the metal lead frame and the reflector 4, a sealing resin layer 6 for sealing the optical semiconductor element 3 is formed. The sealing resin layer 6 may contain a phosphor as needed. In Fig. 1, 7, 8 are electrically connected to a bonding line of an electrode circuit (not shown) formed on a metal lead frame and the optical semiconductor element 3.
再者，在本發明中，也可以使用各種基板來取代 上述圖1之金屬引線框。作為上述各種基板，可舉有機基板、無機基板、撓性印刷基板等為例。又，也可變更轉移成形，藉由射出成形形成反射器。 Furthermore, in the present invention, various substrates can also be used instead. The metal lead frame of Figure 1 above. Examples of the various substrates described above include an organic substrate, an inorganic substrate, and a flexible printed circuit board. Further, the transfer molding may be changed, and the reflector may be formed by injection molding.
又，作為與上述構成相異之光半導體裝置，可舉使用了板狀光半導體裝置用引線框、例如圖2及圖3(圖2之X-X’箭頭指向截面圖)所示之光半導體裝置為例。亦即，該光半導體裝置做成以下構成：在互設間隔配置之金屬引線框10之厚度方向上一面的預定位置，分別裝載有光半導體元件3，且在上述金屬引線框10間的間隙形成有由本發明之熱硬化性樹脂組成物構成的光反射用反射器11。又，如圖3所示，在金屬引線框10之與光半導體元件3裝載面為相反之面上，於多數個地方形成有將本發明之熱硬化性樹脂組成物填充且經硬化而成之反射器11。再者，在圖2及圖3中，12為電性連接上述光半導體元件3與金屬引線框10的接合線。此種光半導體裝置是將上述金屬引線框10設置於轉移成形機之模具內，藉由轉移成形，在設有間隔配置之金屬引線框10的間隙以及形成於金屬引線框10之與光半導體元件3裝載面為相反之面的凹部中，填充熱硬化性樹脂組成物並使其硬化，而分別形成反射器11。接下來，將光半導體元件3裝載在上述金屬引線框10之成為預定位置的光半導體元件裝載區域後，使用接合線12電性連接光半導體元件3與金屬引線框10。如此進行，即可製作出圖2及圖3所示之光半導體裝置。 Further, as an optical semiconductor device different from the above-described configuration, a lead frame for a plate-shaped optical semiconductor device, for example, an optical semiconductor as shown in FIGS. 2 and 3 (X-X' arrow pointing cross-sectional view) is used. The device is taken as an example. In other words, the optical semiconductor device has a configuration in which the optical semiconductor element 3 is mounted on a predetermined position on one surface in the thickness direction of the metal lead frame 10 which is disposed at intervals, and is formed in a gap between the metal lead frames 10. There is a reflector 11 for light reflection which is composed of a thermosetting resin composition of the present invention. Further, as shown in FIG. 3, the thermosetting resin composition of the present invention is filled and hardened in a plurality of places on the surface of the metal lead frame 10 opposite to the surface on which the optical semiconductor element 3 is mounted. Reflector 11. Further, in FIGS. 2 and 3, reference numeral 12 denotes a bonding wire electrically connecting the optical semiconductor element 3 and the metal lead frame 10. In the optical semiconductor device, the metal lead frame 10 is placed in a mold of a transfer molding machine, and a gap between the metal lead frame 10 and the metal lead frame 10 and the optical semiconductor element formed in the metal lead frame 10 are formed by transfer molding. In the recessed portion in which the loading surface is the opposite surface, the thermosetting resin composition is filled and hardened, and the reflector 11 is formed separately. Next, after the optical semiconductor element 3 is mounted on the optical semiconductor element mounting region of the metal lead frame 10 at a predetermined position, the optical semiconductor element 3 and the metal lead frame 10 are electrically connected by using the bonding wires 12. In this way, the optical semiconductor device shown in FIGS. 2 and 3 can be produced.
接著，將實施例與比較例一起說明。然而，本發明並不受限於這些實施例。 Next, the examples will be described together with the comparative examples. However, the invention is not limited to these examples.
首先，在製作熱硬化性樹脂組成物之前，準備如下所示之各成分。 First, each component shown below is prepared before the thermosetting resin composition is produced.
[環氧樹脂] [Epoxy resin]
異三聚氰酸三環氧丙酯(環氧當量100) Triglycidyl isocyanurate (epoxy equivalent 100)
[矽氧樹脂a1] [矽 树脂 a1]
信越化學工業公司製，KER-2500(二液型：混合A液、B液而使用) Shin-Etsu Chemical Co., Ltd., KER-2500 (two-liquid type: mixed with liquid A and liquid B)
[矽氧樹脂a2] [矽 树脂 a2]
信越化學工業公司製，SCR-1012(二液型：混合A液、B液而使用) Shin-Etsu Chemical Co., Ltd., SCR-1012 (two-liquid type: mixed with liquid A and liquid B)
[硬化劑] [hardener]
4-甲基六氫鄰苯二甲酐(x)與六氫鄰苯二甲酐(y)的混合物(液體，混合重量比x/y=70/30)(新日本理化公司製，Rikasid MH-700) a mixture of 4-methylhexahydrophthalic anhydride (x) and hexahydrophthalic anhydride (y) (liquid, mixed weight ratio x/y = 70/30) (Rikasid MH, manufactured by Nippon Chemical and Chemical Co., Ltd.) -700)
[氧化鋯c1] [Zirconium oxide c1]
第一稀元素化學工業公司製，SG氧化鋯，平均粒徑4.3μm Made of the first dilute element chemical industry company, SG zirconia, average particle size 4.3μm
[氧化鋯c2] [zirconia c2]
第一稀元素化學工業公司製，UEP氧化鋯，平均粒徑0.5μm First rare element chemical industry company, UEP zirconia, average particle size 0.5μm
[硬化促進劑] [hardening accelerator]
甲基三丁鏻二甲磷酸鹽(日本化學工業公司製， HISHIKOLIN PX-4MP) Methyl tributyl dimethyl phosphate (manufactured by Nippon Chemical Industry Co., Ltd.) HISHIKOLIN PX-4MP)
[氧化鈦] [titanium oxide]
DuPont公司製，R706，單一粒子徑0.31μm Made by DuPont, R706, single particle diameter 0.31μm
[氧化鋅] [Zinc oxide]
Hakusui Tech Co.,Ltd製，氧化鋅(1種) Manufactured by Hakusui Tech Co., Ltd., zinc oxide (1 species)
[無機質填充劑] [Inorganic filler]
熔融球狀二氧化矽粉末(平均粒徑20μm) Melted spherical cerium oxide powder (average particle size 20 μm)
[實施例1~10，比較例1~16] [Examples 1 to 10, Comparative Examples 1 to 16]
將後述表1~表3所示之各成分以同表所示之比例摻混，並進行藉混煉機施行之熔融混煉(溫度100~130℃)，在熟成之後，冷卻到室溫(25℃)並粉碎，藉此製成作為目的之粉末狀熱硬化性樹脂組成物。 Each component shown in Tables 1 to 3 described later is blended at a ratio shown in the same table, and melt-kneaded by a kneader (temperature: 100 to 130 ° C), and after cooling, it is cooled to room temperature ( 25 ° C) and pulverized, thereby producing a powdery thermosetting resin composition as a target.
使用如此進行而製得之實施例以及比較例的熱硬化性樹脂組成物，依據下述之方法進行光反射率(波長：365nm，405nm，450nm)之測量。其結果顯示於後述之表1~表3中。 Using the thermosetting resin composition of the examples and the comparative examples obtained in this manner, the light reflectance (wavelength: 365 nm, 405 nm, 450 nm) was measured in accordance with the method described below. The results are shown in Tables 1 to 3 which will be described later.
[光反射率] [light reflectance]
使用上述各熱硬化性樹脂組成物，利用預定之硬化條件(條件：175℃×2分鐘的成形+175℃×3小時硬化)製作厚度1mm的試驗片，使用該試驗片(硬化物)，測量在室溫(25℃)下的各光反射率(365nm，405nm，450nm)。再者，測量時，使用日本分光公司製的分光光度計V-670，在室溫(25℃)下測量各波長(365nm，405nm，450nm)之光反射率。 Using each of the above thermosetting resin compositions, a test piece having a thickness of 1 mm was produced by using predetermined curing conditions (condition: 175 ° C × 2 minutes of molding + 175 ° C × 3 hours of hardening), and the test piece (cured product) was used for measurement. Light reflectance (365 nm, 405 nm, 450 nm) at room temperature (25 ° C). Further, at the time of measurement, the light reflectance of each wavelength (365 nm, 405 nm, 450 nm) was measured at room temperature (25 ° C) using a spectrophotometer V-670 manufactured by JASCO Corporation.
從上述結果看出，僅使用氧化鋯作為白色顏料而成之實施例樣品，可得到對各波長(365nm，405nm，450nm)之光具有高的光反射率之優異結果。 From the above results, it was found that the sample of the example using only zirconia as a white pigment gave excellent results of high light reflectance for light of each wavelength (365 nm, 405 nm, 450 nm).
相對於此，除氧化鋯外還摻混少量之氧化鈦或氧化鋅作為白色顏料而成的比較例樣品，可得到特別對波長365nm之光的光反射率明顯降低的結果。 On the other hand, in the case of a comparative example in which a small amount of titanium oxide or zinc oxide was added as a white pigment in addition to zirconia, the light reflectance of light having a wavelength of 365 nm was remarkably lowered.
[光半導體(發光)裝置之製作] [Production of Optical Semiconductor (Light Emitting) Device]
接著，使用上述實施例樣品之粉末狀熱硬化性樹脂組成物，製造出圖1所示之構成的光半導體(發光)裝置。亦即，將具有數對銅(鍍銀)製之第1板部1與第2板部2的金屬引線框設置於轉移成形機的模具內，使用上述熱硬化性樹脂組 成物來進行轉移成形(條件：175℃×2分鐘的成形+175℃×3小時硬化)，藉以如圖1所示，在金屬引線框面之預定位置形成反射器4。接著，裝載光半導體(發光)元件(大小1mm×1mm，發光波長：395-400nm)3，並藉由接合線7、8電性連接此光半導體元件3與上述金屬引線框，以製造出具備有反射器4、金屬引線框與光半導體元件3之單元。 Next, using the powdery thermosetting resin composition of the sample of the above example, an optical semiconductor (light-emitting) device having the configuration shown in Fig. 1 was produced. In other words, a metal lead frame having a plurality of pairs of copper (silver-plated) first plate portions 1 and second plate portions 2 is placed in a mold of a transfer molding machine, and the above-mentioned thermosetting resin group is used. The object was subjected to transfer molding (condition: 175 ° C × 2 minutes of formation + 175 ° C × 3 hours of hardening), whereby the reflector 4 was formed at a predetermined position on the metal lead frame surface as shown in FIG. Next, a photo-semiconductor (light-emitting) device (having a size of 1 mm × 1 mm, an emission wavelength: 395 to 400 nm) 3 is mounted, and the optical semiconductor element 3 and the metal lead frame are electrically connected by bonding wires 7 and 8 to be manufactured. There is a unit of the reflector 4, the metal lead frame and the optical semiconductor element 3.
其次，在上述金屬引線框與反射器4的內周面所形成之凹部5中，藉由填充矽氧樹脂(信越Silicone公司製，KER-2500)，對上述光半導體元件3進行樹脂密封(成形條件：150℃×4小時)以形成透明的密封樹脂層6，且就每一個反射器進行切割使其單片化，製作出圖1所示之光半導體(發光)裝置。所製得之光半導體(發光)裝置為，可得到具備高的光反射率，且具有高可靠性之良好的光半導體(發光)裝置。 Next, in the recessed portion 5 formed on the inner peripheral surface of the metal lead frame and the reflector 4, the optical semiconductor element 3 is resin-sealed (formed by filling with a silicone resin (KER-2500, manufactured by Shin-Etsu Silicone Co., Ltd.). Condition: 150 ° C × 4 hours) to form a transparent sealing resin layer 6, and each of the reflectors was cut and singulated to fabricate the optical semiconductor (light-emitting) device shown in FIG. The obtained photo-semiconductor (light-emitting) device is capable of obtaining a good optical semiconductor (light-emitting) device having high light reflectance and high reliability.
在上述實施例中，顯示本發明之具體形態，但是上述實施例僅為舉例說明，並非用以限定地解釋。且對所屬技術領域中具有通常知識者來說是明顯的各種變形，皆在本發明的範圍內。 In the above embodiments, the specific embodiments of the present invention are shown, but the above embodiments are merely illustrative and are not to be construed as limiting. It is obvious to those skilled in the art that various modifications are possible within the scope of the invention.
本發明之光半導體裝置用熱硬化性樹脂組成物，作為使內建於光半導體裝置中之光半導體元件發出之波長350~410nm的光反射之反射器形成材料是有用的。 The thermosetting resin composition for an optical semiconductor device of the present invention is useful as a reflector forming material for reflecting light having a wavelength of 350 to 410 nm emitted from an optical semiconductor element built in an optical semiconductor device.
1‧‧‧第1板部 1‧‧‧1st Board
2‧‧‧第2板部 2‧‧‧2nd Board
3‧‧‧光半導體元件 3‧‧‧Optical semiconductor components
4‧‧‧反射器 4‧‧‧ reflector
5‧‧‧凹部 5‧‧‧ recess
6‧‧‧密封樹脂層 6‧‧‧ sealing resin layer
7、8‧‧‧接合線 7,8‧‧‧bonding line
Claims (11)
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
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| JP2013251258A JP2015109337A (en) | 2013-12-04 | 2013-12-04 | Thermosetting resin composition for optical semiconductor devices, lead frame for optical semiconductor devices obtained by using the same, and optical semiconductor device |
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| Publication Number | Publication Date |
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| TW201527380A true TW201527380A (en) | 2015-07-16 |
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| TW103140781A TW201527380A (en) | 2013-12-04 | 2014-11-25 | Heat-curable resin composition for optical semiconductor device, lead frame for optical semiconductor device and obtained using same, and optical semiconductor device |
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| JP (1) | JP2015109337A (en) |
| KR (1) | KR20160094368A (en) |
| CN (1) | CN105594004A (en) |
| TW (1) | TW201527380A (en) |
| WO (1) | WO2015083576A1 (en) |
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| CN108136662B (en) | 2015-09-03 | 2021-08-06 | 美国陶氏有机硅公司 | 3D printing method using heat-curable silicone composition |
| KR20180128921A (en) * | 2016-03-30 | 2018-12-04 | 히타치가세이가부시끼가이샤 | Thermosetting resin composition, substrate for mounting optical semiconductor element, manufacturing method thereof, and optical semiconductor device |
| JP7053980B2 (en) * | 2016-11-16 | 2022-04-13 | 日亜化学工業株式会社 | Light emitting device |
| CN115667418A (en) | 2020-05-19 | 2023-01-31 | 毕克化学有限公司 | Thermosetting polymer powder |
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| JP2005306952A (en) * | 2004-04-20 | 2005-11-04 | Japan Epoxy Resin Kk | Epoxy resin composition as sealing material for light-emitting element |
| JP4873963B2 (en) * | 2006-02-27 | 2012-02-08 | 京セラ株式会社 | LIGHT EMITTING DEVICE AND LIGHTING DEVICE USING THE SAME |
| WO2008059856A1 (en) * | 2006-11-15 | 2008-05-22 | Hitachi Chemical Co., Ltd. | Heat curable resin composition for light reflection, process for producing the resin composition, and optical semiconductor element mounting substrate and optical semiconductor device using the resin composition |
| DE102009058006B4 (en) * | 2009-12-11 | 2022-03-31 | OSRAM Opto Semiconductors Gesellschaft mit beschränkter Haftung | Optoelectronic semiconductor component |
| JP2011249768A (en) * | 2010-04-27 | 2011-12-08 | Mitsubishi Chemicals Corp | Semiconductor light-emitting element support member and semiconductor light-emitting device |
| JP5721969B2 (en) | 2010-06-11 | 2015-05-20 | 日東電工株式会社 | Epoxy resin composition for reflector of optical semiconductor device, lead frame for optical semiconductor device obtained using the same, and optical semiconductor device |
| DE102010026344A1 (en) * | 2010-07-07 | 2012-01-12 | Osram Opto Semiconductors Gmbh | led |
| JP5670249B2 (en) * | 2011-04-14 | 2015-02-18 | 日東電工株式会社 | Light emitting element transfer sheet manufacturing method, light emitting device manufacturing method, light emitting element transfer sheet, and light emitting device |
| JP5764423B2 (en) * | 2011-08-02 | 2015-08-19 | 日東電工株式会社 | Epoxy resin composition for optical semiconductor device, lead frame for optical semiconductor device or substrate for optical semiconductor device obtained by using the same, and optical semiconductor device |
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| WO2015083576A1 (en) | 2015-06-11 |
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