JP2006348070A - Oxynitride-based phosphor and method for producing the same - Google Patents
Oxynitride-based phosphor and method for producing the same Download PDFInfo
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- JP2006348070A JP2006348070A JP2005172282A JP2005172282A JP2006348070A JP 2006348070 A JP2006348070 A JP 2006348070A JP 2005172282 A JP2005172282 A JP 2005172282A JP 2005172282 A JP2005172282 A JP 2005172282A JP 2006348070 A JP2006348070 A JP 2006348070A
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- oxides
- nitrides
- elements
- phosphor
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 title claims abstract description 83
- 238000004519 manufacturing process Methods 0.000 title claims description 8
- 150000004767 nitrides Chemical class 0.000 claims abstract description 93
- 229910052693 Europium Inorganic materials 0.000 claims abstract description 25
- 229910052748 manganese Inorganic materials 0.000 claims abstract description 21
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 20
- 229910052692 Dysprosium Inorganic materials 0.000 claims abstract description 20
- 229910052691 Erbium Inorganic materials 0.000 claims abstract description 20
- 229910052689 Holmium Inorganic materials 0.000 claims abstract description 20
- 229910052779 Neodymium Inorganic materials 0.000 claims abstract description 20
- 229910052777 Praseodymium Inorganic materials 0.000 claims abstract description 20
- 229910052772 Samarium Inorganic materials 0.000 claims abstract description 20
- 229910052771 Terbium Inorganic materials 0.000 claims abstract description 20
- 229910052775 Thulium Inorganic materials 0.000 claims abstract description 20
- 229910052787 antimony Inorganic materials 0.000 claims abstract description 20
- 229910052804 chromium Inorganic materials 0.000 claims abstract description 20
- 229910052745 lead Inorganic materials 0.000 claims abstract description 20
- 229910052688 Gadolinium Inorganic materials 0.000 claims abstract description 18
- 229910052727 yttrium Inorganic materials 0.000 claims abstract description 18
- 229910052769 Ytterbium Inorganic materials 0.000 claims abstract description 17
- 239000012190 activator Substances 0.000 claims abstract description 16
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 15
- 229910052706 scandium Inorganic materials 0.000 claims abstract description 15
- 150000001875 compounds Chemical class 0.000 claims description 73
- 238000010438 heat treatment Methods 0.000 claims description 50
- 229910052799 carbon Inorganic materials 0.000 claims description 47
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 42
- 229910052788 barium Inorganic materials 0.000 claims description 25
- 229910052712 strontium Inorganic materials 0.000 claims description 24
- 229910052791 calcium Inorganic materials 0.000 claims description 22
- 229910052710 silicon Inorganic materials 0.000 claims description 21
- 229910052749 magnesium Inorganic materials 0.000 claims description 20
- 229910052790 beryllium Inorganic materials 0.000 claims description 19
- 239000012298 atmosphere Substances 0.000 claims description 17
- 229910052732 germanium Inorganic materials 0.000 claims description 17
- 229910052718 tin Inorganic materials 0.000 claims description 17
- 229910052719 titanium Inorganic materials 0.000 claims description 17
- 229910052726 zirconium Inorganic materials 0.000 claims description 17
- 229910052735 hafnium Inorganic materials 0.000 claims description 16
- 239000004065 semiconductor Substances 0.000 claims description 16
- 230000001590 oxidative effect Effects 0.000 claims description 15
- 229910052792 caesium Inorganic materials 0.000 claims description 11
- 229910052744 lithium Inorganic materials 0.000 claims description 11
- 229910052700 potassium Inorganic materials 0.000 claims description 11
- 229910052701 rubidium Inorganic materials 0.000 claims description 11
- 229910052708 sodium Inorganic materials 0.000 claims description 11
- 239000000463 material Substances 0.000 claims description 7
- 230000003647 oxidation Effects 0.000 claims description 4
- 238000007254 oxidation reaction Methods 0.000 claims description 4
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- 238000002156 mixing Methods 0.000 description 16
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- -1 nitride compound Chemical class 0.000 description 13
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- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 12
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- 239000013078 crystal Substances 0.000 description 9
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- AEBZCFFCDTZXHP-UHFFFAOYSA-N europium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Eu+3].[Eu+3] AEBZCFFCDTZXHP-UHFFFAOYSA-N 0.000 description 7
- 239000010439 graphite Substances 0.000 description 7
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- 239000006104 solid solution Substances 0.000 description 7
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 6
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- 239000001301 oxygen Substances 0.000 description 6
- 239000002245 particle Substances 0.000 description 6
- OGPBJKLSAFTDLK-UHFFFAOYSA-N europium atom Chemical compound [Eu] OGPBJKLSAFTDLK-UHFFFAOYSA-N 0.000 description 5
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 5
- 239000007787 solid Substances 0.000 description 5
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 4
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 4
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 4
- 239000002131 composite material Substances 0.000 description 4
- 150000004679 hydroxides Chemical class 0.000 description 4
- BDAGIHXWWSANSR-NJFSPNSNSA-N hydroxyformaldehyde Chemical compound O[14CH]=O BDAGIHXWWSANSR-NJFSPNSNSA-N 0.000 description 4
- 150000002739 metals Chemical class 0.000 description 4
- 239000010703 silicon Substances 0.000 description 4
- LIVNPJMFVYWSIS-UHFFFAOYSA-N silicon monoxide Chemical compound [Si-]#[O+] LIVNPJMFVYWSIS-UHFFFAOYSA-N 0.000 description 4
- 229910000018 strontium carbonate Inorganic materials 0.000 description 4
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 3
- 238000010521 absorption reaction Methods 0.000 description 3
- 150000001242 acetic acid derivatives Chemical class 0.000 description 3
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- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 3
- 150000002823 nitrates Chemical class 0.000 description 3
- 239000012299 nitrogen atmosphere Substances 0.000 description 3
- 150000002902 organometallic compounds Chemical class 0.000 description 3
- 150000003891 oxalate salts Chemical class 0.000 description 3
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 3
- 239000002002 slurry Substances 0.000 description 3
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 229910002601 GaN Inorganic materials 0.000 description 2
- CSNNHWWHGAXBCP-UHFFFAOYSA-L Magnesium sulfate Chemical compound [Mg+2].[O-][S+2]([O-])([O-])[O-] CSNNHWWHGAXBCP-UHFFFAOYSA-L 0.000 description 2
- BOTDANWDWHJENH-UHFFFAOYSA-N Tetraethyl orthosilicate Chemical compound CCO[Si](OCC)(OCC)OCC BOTDANWDWHJENH-UHFFFAOYSA-N 0.000 description 2
- IWOUKMZUPDVPGQ-UHFFFAOYSA-N barium nitrate Chemical compound [Ba+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O IWOUKMZUPDVPGQ-UHFFFAOYSA-N 0.000 description 2
- QVQLCTNNEUAWMS-UHFFFAOYSA-N barium oxide Chemical compound [Ba]=O QVQLCTNNEUAWMS-UHFFFAOYSA-N 0.000 description 2
- TZCXTZWJZNENPQ-UHFFFAOYSA-L barium sulfate Chemical compound [Ba+2].[O-]S([O-])(=O)=O TZCXTZWJZNENPQ-UHFFFAOYSA-L 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 description 2
- RFVVBBUVWAIIBT-UHFFFAOYSA-N beryllium nitrate Chemical compound [Be+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O RFVVBBUVWAIIBT-UHFFFAOYSA-N 0.000 description 2
- KQHXBDOEECKORE-UHFFFAOYSA-L beryllium sulfate Chemical compound [Be+2].[O-]S([O-])(=O)=O KQHXBDOEECKORE-UHFFFAOYSA-L 0.000 description 2
- ZCCIPPOKBCJFDN-UHFFFAOYSA-N calcium nitrate Chemical compound [Ca+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O ZCCIPPOKBCJFDN-UHFFFAOYSA-N 0.000 description 2
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 2
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- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
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- 229920001971 elastomer Polymers 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- XGZVUEUWXADBQD-UHFFFAOYSA-L lithium carbonate Chemical compound [Li+].[Li+].[O-]C([O-])=O XGZVUEUWXADBQD-UHFFFAOYSA-L 0.000 description 2
- YIXJRHPUWRPCBB-UHFFFAOYSA-N magnesium nitrate Chemical compound [Mg+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O YIXJRHPUWRPCBB-UHFFFAOYSA-N 0.000 description 2
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- DHEQXMRUPNDRPG-UHFFFAOYSA-N strontium nitrate Chemical compound [Sr+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O DHEQXMRUPNDRPG-UHFFFAOYSA-N 0.000 description 2
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- UQMOLLPKNHFRAC-UHFFFAOYSA-N tetrabutyl silicate Chemical compound CCCCO[Si](OCCCC)(OCCCC)OCCCC UQMOLLPKNHFRAC-UHFFFAOYSA-N 0.000 description 2
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- GIRKRMUMWJFNRI-UHFFFAOYSA-N tris(dimethylamino)silicon Chemical compound CN(C)[Si](N(C)C)N(C)C GIRKRMUMWJFNRI-UHFFFAOYSA-N 0.000 description 2
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- FRWYFWZENXDZMU-UHFFFAOYSA-N 2-iodoquinoline Chemical compound C1=CC=CC2=NC(I)=CC=C21 FRWYFWZENXDZMU-UHFFFAOYSA-N 0.000 description 1
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- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- 101100286286 Dictyostelium discoideum ipi gene Proteins 0.000 description 1
- JMASRVWKEDWRBT-UHFFFAOYSA-N Gallium nitride Chemical compound [Ga]#N JMASRVWKEDWRBT-UHFFFAOYSA-N 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 229910002651 NO3 Inorganic materials 0.000 description 1
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 1
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- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- NRTOMJZYCJJWKI-UHFFFAOYSA-N Titanium nitride Chemical compound [Ti]#N NRTOMJZYCJJWKI-UHFFFAOYSA-N 0.000 description 1
- PILWPTAXXILTMN-UHFFFAOYSA-N [Ar].O=[C] Chemical compound [Ar].O=[C] PILWPTAXXILTMN-UHFFFAOYSA-N 0.000 description 1
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- 229910001508 alkali metal halide Inorganic materials 0.000 description 1
- 150000008045 alkali metal halides Chemical class 0.000 description 1
- 229910001615 alkaline earth metal halide Inorganic materials 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- PSBUJOCDKOWAGJ-UHFFFAOYSA-N azanylidyneeuropium Chemical compound [Eu]#N PSBUJOCDKOWAGJ-UHFFFAOYSA-N 0.000 description 1
- AJXBBNUQVRZRCZ-UHFFFAOYSA-N azanylidyneyttrium Chemical compound [Y]#N AJXBBNUQVRZRCZ-UHFFFAOYSA-N 0.000 description 1
- ITHZDDVSAWDQPZ-UHFFFAOYSA-L barium acetate Chemical compound [Ba+2].CC([O-])=O.CC([O-])=O ITHZDDVSAWDQPZ-UHFFFAOYSA-L 0.000 description 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 description 1
- RQPZNWPYLFFXCP-UHFFFAOYSA-L barium dihydroxide Chemical compound [OH-].[OH-].[Ba+2] RQPZNWPYLFFXCP-UHFFFAOYSA-L 0.000 description 1
- 229910001863 barium hydroxide Inorganic materials 0.000 description 1
- GXUARMXARIJAFV-UHFFFAOYSA-L barium oxalate Chemical compound [Ba+2].[O-]C(=O)C([O-])=O GXUARMXARIJAFV-UHFFFAOYSA-L 0.000 description 1
- 229940094800 barium oxalate Drugs 0.000 description 1
- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 description 1
- 229910002113 barium titanate Inorganic materials 0.000 description 1
- TVSNZOUKUFGNLK-UHFFFAOYSA-N barium(2+);butan-1-olate Chemical compound [Ba+2].CCCC[O-].CCCC[O-] TVSNZOUKUFGNLK-UHFFFAOYSA-N 0.000 description 1
- GYIWFHXWLCXGQO-UHFFFAOYSA-N barium(2+);ethanolate Chemical compound [Ba+2].CC[O-].CC[O-] GYIWFHXWLCXGQO-UHFFFAOYSA-N 0.000 description 1
- BQDSDRAVKYTTTH-UHFFFAOYSA-N barium(2+);methanolate Chemical compound [Ba+2].[O-]C.[O-]C BQDSDRAVKYTTTH-UHFFFAOYSA-N 0.000 description 1
- AYJRCSIUFZENHW-DEQYMQKBSA-L barium(2+);oxomethanediolate Chemical compound [Ba+2].[O-][14C]([O-])=O AYJRCSIUFZENHW-DEQYMQKBSA-L 0.000 description 1
- ZCKXRHNLRWLPLJ-UHFFFAOYSA-N barium(2+);propan-1-olate Chemical compound [Ba+2].CCC[O-].CCC[O-] ZCKXRHNLRWLPLJ-UHFFFAOYSA-N 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- ZBUQRSWEONVBES-UHFFFAOYSA-L beryllium carbonate Chemical compound [Be+2].[O-]C([O-])=O ZBUQRSWEONVBES-UHFFFAOYSA-L 0.000 description 1
- 229910000023 beryllium carbonate Inorganic materials 0.000 description 1
- WPJWIROQQFWMMK-UHFFFAOYSA-L beryllium dihydroxide Chemical compound [Be+2].[OH-].[OH-] WPJWIROQQFWMMK-UHFFFAOYSA-L 0.000 description 1
- 229910001865 beryllium hydroxide Inorganic materials 0.000 description 1
- LTPBRCUWZOMYOC-UHFFFAOYSA-N beryllium oxide Inorganic materials O=[Be] LTPBRCUWZOMYOC-UHFFFAOYSA-N 0.000 description 1
- YUOUKRIPFJKDJY-UHFFFAOYSA-L beryllium;diacetate Chemical compound [Be+2].CC([O-])=O.CC([O-])=O YUOUKRIPFJKDJY-UHFFFAOYSA-L 0.000 description 1
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- WFIQYLBVIPISPT-UHFFFAOYSA-N butan-1-olate europium(3+) Chemical compound [Eu+3].CCCC[O-].CCCC[O-].CCCC[O-] WFIQYLBVIPISPT-UHFFFAOYSA-N 0.000 description 1
- PCOPFSXTYFFNIG-UHFFFAOYSA-N butan-1-olate;yttrium(3+) Chemical compound [Y+3].CCCC[O-].CCCC[O-].CCCC[O-] PCOPFSXTYFFNIG-UHFFFAOYSA-N 0.000 description 1
- 238000001354 calcination Methods 0.000 description 1
- VSGNNIFQASZAOI-UHFFFAOYSA-L calcium acetate Chemical compound [Ca+2].CC([O-])=O.CC([O-])=O VSGNNIFQASZAOI-UHFFFAOYSA-L 0.000 description 1
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- JHLCADGWXYCDQA-UHFFFAOYSA-N calcium;ethanolate Chemical compound [Ca+2].CC[O-].CC[O-] JHLCADGWXYCDQA-UHFFFAOYSA-N 0.000 description 1
- AMJQWGIYCROUQF-UHFFFAOYSA-N calcium;methanolate Chemical compound [Ca+2].[O-]C.[O-]C AMJQWGIYCROUQF-UHFFFAOYSA-N 0.000 description 1
- OEPJXTZQPRTGCX-UHFFFAOYSA-N calcium;propan-1-olate Chemical compound [Ca+2].CCC[O-].CCC[O-] OEPJXTZQPRTGCX-UHFFFAOYSA-N 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
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- 230000000295 complement effect Effects 0.000 description 1
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- RAABOESOVLLHRU-UHFFFAOYSA-N diazene Chemical compound N=N RAABOESOVLLHRU-UHFFFAOYSA-N 0.000 description 1
- 229910000071 diazene Inorganic materials 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 239000000806 elastomer Substances 0.000 description 1
- CCUCUHRUAPGBHB-UHFFFAOYSA-N ethanolate europium(3+) Chemical compound [Eu+3].CC[O-].CC[O-].CC[O-] CCUCUHRUAPGBHB-UHFFFAOYSA-N 0.000 description 1
- KEQVPIDOPAGWCP-UHFFFAOYSA-N ethanolate;yttrium(3+) Chemical compound [Y+3].CC[O-].CC[O-].CC[O-] KEQVPIDOPAGWCP-UHFFFAOYSA-N 0.000 description 1
- SULCVUWEGVSCPF-UHFFFAOYSA-L europium(2+);carbonate Chemical compound [Eu+2].[O-]C([O-])=O SULCVUWEGVSCPF-UHFFFAOYSA-L 0.000 description 1
- LTCGYPJIBNZNSY-UHFFFAOYSA-N europium(3+) methanolate Chemical compound [Eu+3].[O-]C.[O-]C.[O-]C LTCGYPJIBNZNSY-UHFFFAOYSA-N 0.000 description 1
- PVDYMOCCGHXJAK-UHFFFAOYSA-H europium(3+);oxalate Chemical compound [Eu+3].[Eu+3].[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O.[O-]C(=O)C([O-])=O PVDYMOCCGHXJAK-UHFFFAOYSA-H 0.000 description 1
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- CQQZFSZWNXAJQN-UHFFFAOYSA-K europium(3+);trihydroxide Chemical compound [OH-].[OH-].[OH-].[Eu+3] CQQZFSZWNXAJQN-UHFFFAOYSA-K 0.000 description 1
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Landscapes
- Luminescent Compositions (AREA)
- Led Device Packages (AREA)
- Led Devices (AREA)
Abstract
Description
æ¬çºæã¯ãåžåé¡å çŽ çã§å åŠçã«æŽ»æ§åãããé žçªåç©ç³»èå äœã«é¢ãããããã«è©³ããã¯ãéè²çºå ãã€ãªãŒã(éè²ïŒ¬ïŒ¥ïŒ€)ãŸãã¯çŽ«å€çºå ãã€ãªãŒã(玫å€ïŒ¬ïŒ¥ïŒ€)ãå±èµ·å æºãšããŠæ³¢é·å€æããããšãå¯èœãšããé žçªåç©ç³»èå äœã«é¢ããã   The present invention relates to an oxynitride phosphor optically activated with a rare earth element or the like. More specifically, the present invention relates to an oxynitride phosphor that enables wavelength conversion using a blue light emitting diode (blue LED) or an ultraviolet light emitting diode (ultraviolet LED) as an excitation light source.
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A light emitting diode (LED) is a semiconductor solid state light emitting device in which a p-type semiconductor and an n-type semiconductor are joined. LEDs have advantages such as long life, excellent impact resistance, low power consumption, high reliability, and can be reduced in size, thickness, and weight, so they are used as light sources for various devices. Yes. In particular, white LEDs are used for disaster prevention lighting that requires reliability, in-vehicle lighting and liquid crystal backlights that are favored for miniaturization and weight reduction, destination information guides for stations that require visibility, etc. Application to indoor lighting in general households is also expected.
When a current is passed in the forward direction of a pn junction made of a direct transition type semiconductor, electrons and holes are recombined, and light having a peak wavelength corresponding to the forbidden band width of the semiconductor is emitted. Since the emission spectrum of an LED generally has a narrow peak wavelength half-width, the emission color of a white LED is obtained exclusively by the principle of color mixing.
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As a method of obtaining white, specifically,
(1) A method of combining three kinds of LEDs each emitting red (R), green (G) and blue (B), which are the three primary colors of light, and mixing these LED lights,
(2) An ultraviolet LED that emits ultraviolet rays and three types of phosphors that are excited by the ultraviolet rays and emit red (R), green (G), and blue (B) fluorescence, are combined and emitted from the phosphor. To mix the three colors of fluorescence,
(3) A blue LED that emits blue light and a phosphor that is excited by the blue light and emits yellow fluorescence that is complementary to the blue light are combined, and the blue LED light is emitted from the phosphor. How to mix with yellow light,
Etc. are known.
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The method of obtaining a predetermined emission color using a plurality of LEDs requires a special circuit for adjusting the current of each LED in order to balance each color. On the other hand, the method of obtaining a predetermined emission color by combining the LED and the phosphor does not require such a circuit and has an advantage that the cost of the LED can be reduced. Therefore, various proposals have conventionally been made for this type of phosphor using an LED as a light source.
For example, there is disclosed a YAG phosphor in which Ce is doped in a YAG-based oxide base crystal represented by a composition formula of (Y, Gd) 3 (Al, Ga) 5 O 12 (see Non-Patent Document 1). . In this document, the surface of an InGaN blue LED chip is thinly coated with a YAG phosphor, whereby blue light emitted from the blue LED and a peak wavelength 550 nm emitted from the YAG phosphor excited by the blue light are disclosed. It is described that white light can be obtained by mixing with the fluorescence.
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Existing phosphors generally have the disadvantage that the spectral intensity is significantly reduced when the excitation wavelength exceeds the near ultraviolet region.
In addition, a white LED obtained by coating a phosphor surface made of a YAG-based oxide on the surface of an InGaN-based blue LED chip has an excitation energy of a YAG-based oxide that is a phosphor and an excitation energy of a blue LED as a light source. Since the excitation energy is not converted efficiently, it has been considered difficult to produce a high-intensity white LED.
Furthermore, when a light emitting element such as a nitride compound semiconductor capable of emitting ultraviolet light and a phosphor that emits light when excited by ultraviolet light are combined to form a white LED, the luminous efficiency of the red component phosphor is higher than that of other phosphors. However, since the mixing ratio is too high, it has been considered difficult to obtain a high brightness white color.
The present invention relates to an oxynitride phosphor capable of increasing the brightness of a white light emitting diode (white LED) using a blue light emitting diode (blue LED) or an ultraviolet light emitting diode (ultraviolet LED) as a light source, and light emission using the same. An object is to provide an apparatus.
æ¬çºæè ã¯ãäžèšç®çéæã®ããã«éææ€èšããçµæã賊掻å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å çŽ ãçšããããã«Sc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å çŽ ãã¢ã«ã«ãªåé¡éå±å çŽ ãåšæåŸè¡šã®ç¬¬IVå±å çŽ ã第IVå±å çŽ ãå«ãé žçªåç©èå äœã賊掻å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å çŽ ãçšããããã«ã¢ã«ã«ãªéå±ãã¢ã«ã«ãªåé¡éå±å çŽ ãåšæåŸè¡šã®ç¬¬IVå±å çŽ ã第IVå±å çŽ ãå«ãé žçªåç©èå äœåã³è³ŠæŽ»å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å çŽ ãçšããããã«Sc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å çŽ ãã¢ã«ã«ãªéå±ãã¢ã«ã«ãªåé¡éå±å çŽ ãåšæåŸè¡šã®ç¬¬IVå±å çŽ ã第IVå±å çŽ ãå«ãé žçªåç©èå äœãã玫å€ãè¿çŽ«å€ãå¯èŠå ã«ãããåºç¯å²ã®åŒ·ãåžå垯ãæããããšãèŠåºããåœè©²çºå æ³¢é·ãæããLEDå ã«ããå±èµ·ãããæ³¢é·å€æããé·æ³¢é·åŽã®çºå ã瀺ãããšãæ°ãã«èŠåºãæ¬çºæãå®æãããã«è³ã£ãã   As a result of intensive studies for achieving the above-mentioned object, the present inventor is composed of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb in the activator Z. Using at least one element selected from the group, one or more elements selected from the group consisting of Sc, Y, La, Gd, Yb, alkaline earth metal elements, Group IVA elements of the periodic table, The oxynitride phosphor containing the Group IVB element and the activator Z are selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb At least one element is used, and an alkali metal, alkaline earth metal element, group IVA element of the periodic table, oxynitride phosphor containing group IVB element and activator Z, Ce, Pr, Nd , Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb, and at least one element selected from the group consisting of Sc, Y, La, Gd, Yb One or more elements selected from the group consisting of alkali metal, alkaline earth metal element, group IVA element and group IVB in the periodic table The oxynitride phosphor containing silicon has a broad absorption band ranging from ultraviolet to near-ultraviolet to visible light, and is excited by the LED light having the emission wavelength, converts the wavelength, and emits light on the long wavelength side. The inventors have newly found out that the present invention has been completed.
å³ã¡ãæ¬çºæã¯ä»¥äžã®åé
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ïŒïŒïŒ 賊掻å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãçšãããR-L-M-O-NïŒZç³»é
žçªåç©èå
äœãïŒRã¯ãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããLã¯ãBe,Mg,Ca,Sr,Baããããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããMã¯ãC,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããïŒ
ïŒïŒïŒ 賊掻å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãçšãããD-L-M-O-NïŒZç³»é
žçªåç©èå
äœãïŒDã¯ãLi,Na,K,Rb,Csãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ãããLã¯ãBe,Mg,Ca,Sr,Baããããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããMã¯ãC,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããïŒ
ïŒïŒïŒ 賊掻å€Zã«ãCe,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãçšãããD-R-L-M-O-NïŒZç³»é
žçªåç©èå
äœãïŒDã¯ãLi,Na,K,Rb,Csãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ãããRã¯ãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããLã¯ãBe,Mg,Ca,Sr,Baããããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããMã¯ãC,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ãããïŒ
That is, the present invention comprises the inventions of the following items.
(1) As the activator Z, at least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb was used. RLMON: Z-based oxynitride phosphor. (R is one or more elements selected from the group consisting of Sc, Y, La, Gd, Yb, and L is one or more elements selected from the group consisting of Be, Mg, Ca, Sr, Ba) And M is one or more elements selected from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf.)
(2) For the activator Z, at least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb was used. DLMON: Z-based oxynitride phosphor. (D is at least one element selected from the group consisting of Li, Na, K, Rb, and Cs, and L is one or more elements selected from the group consisting of Be, Mg, Ca, Sr, and Ba. And M is one or more elements selected from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf.)
(3) At least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb was used as the activator Z. DRLMON: Z-based oxynitride phosphor. (D is at least one element selected from the group consisting of Li, Na, K, Rb, Cs, and R is one or more elements selected from the group consisting of Sc, Y, La, Gd, Yb. L is one or more elements selected from the group consisting of Be, Mg, Ca, Sr, Ba, and M is from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf. One or more elements selected.)
ïŒïŒïŒ Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãBe,Mg,Ca,Sr,Baã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãCïŒæãã¯Si,Ge,Sn,Ti,Zr,Hfã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ãšãæ··åããç空ãããã¯éé
žåæ§é°å²æ°äžïŒïŒïŒãïŒïŒïŒïŒâã§çŒæããããšãç¹åŸŽãšããäžèšïŒïŒïŒã«èšèŒã®é
žçªåç©ç³»èå
äœã®è£œé æ³ã
ïŒïŒïŒ Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãLi,Na,K,Rb,Csã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãBe,Mg,Ca,Sr,Baã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãCãæãã¯Si,Ge,Sn,Ti,Zr,Hfã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãæ··åããç空ãããã¯éé
žåæ§é°å²æ°äžïŒïŒïŒãïŒïŒïŒïŒâã§çŒæããããšãç¹åŸŽãšããäžèšïŒïŒïŒã«èšèŒã®é
žçªåç©ç³»èå
äœã®è£œé æ³ã
(4) At least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb, oxide, nitride, or by heating At least one of these oxides and nitride forming compounds and one or more elements selected from the group consisting of Sc, Y, La, Gd, Yb, oxides, nitrides, or these oxides by heating, At least one of compounds forming nitride, at least one of elements of Be, Mg, Ca, Sr, Ba, oxides, nitrides or these oxides and nitrides by heating, C, or Si, Ge, Sn, Ti, Zr, Hf elements, oxides, nitrides, or these oxides and compounds that form nitrides by mixing with heat, mixed in a vacuum or non-oxidizing atmosphere at 900-1900 ° C. The method for producing an oxynitride phosphor according to (1) above, characterized by firing.
(5) At least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb, oxide, nitride, or by heating At least one of these oxides and nitride forming compounds and at least one of Li, Na, K, Rb and Cs elements, oxides, nitrides, or compounds that form these oxides and nitrides by heating And at least one of the elements of Be, Mg, Ca, Sr, Ba, oxides, nitrides, or compounds that form these oxides and nitrides by heating, and C, or Si, Ge, Sn, Ti, Zr , Hf elements, oxides, nitrides, or at least one of these oxides and nitride-forming compounds mixed with heat, and fired at 900 to 1900 ° C. in a vacuum or non-oxidizing atmosphere. The method for producing an oxynitride phosphor according to (2) above.
ïŒïŒïŒ Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãLi,Na,K,Rb,Csã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãBe,Mg,Ca,Sr,Baã®å
çŽ ãé
žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãCãæãã¯Si,Ge,Sn,Ti,Zr,Hfã®å
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žåç©ãçªåç©æãã¯å ç±ã«ãããããã®é
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(6) At least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb, oxide, nitride, or by heating At least one of these oxides and nitride forming compounds and one or more elements selected from the group consisting of Sc, Y, La, Gd, Yb, oxides, nitrides, or these oxides by heating, At least one compound that forms nitrides, at least one of Li, Na, K, Rb, and Cs elements, oxides, nitrides, or compounds that form these oxides and nitrides by heating, Be, Mg , Ca, Sr, Ba elements, oxides, nitrides, or at least one of these oxides, nitride-forming compounds, and C, Si, Ge, Sn, Ti, Zr, Hf elements, A vacuum or non-oxidizing atmosphere in which at least one of oxides, nitrides or compounds that form oxides or nitrides by heating is mixed with carbon. The method for producing an oxynitride phosphor according to the above (3), characterized by firing at 900 to 1900 ° C.
(7) A light emitting device in which the oxynitride phosphor according to (1) to (3) above and a light emitting element are combined.
(8) The light-emitting device according to (7), wherein the light-emitting element is a nitride-based semiconductor light-emitting element, and the light emission wavelength of the light-emitting element is in the range of 250 nm to 500 nm.
æ¬çºæã®èå äœã¯ã玫å€ãè¿çŽ«å€ãå¯èŠå ã«ãããåºç¯å²ã®åžå垯ãæããããšããã玫å€ïŒ¬ïŒ¥ïŒ€ãéè²ïŒ¬ïŒ¥ïŒ€ãçšããå ã®æ³¢é·å€æã«æå¹ã«é©çšããããšãã§ããããŸããåžå垯ã匷ãããšãããç¹ã«çœè²ïŒ¬ïŒ¥ïŒ€çšéã«æå¹ã«é©çšããããšãå¯èœã§ãããçœè²ïŒ¬ïŒ¥ïŒ€ã®èŒåºŠãåäžãããããšãã§ããã   Since the phosphor of the present invention has a wide absorption band ranging from ultraviolet to near ultraviolet to visible light, it can be effectively applied to wavelength conversion of LED light using an ultraviolet LED or a blue LED. Moreover, since the absorption band is strong, it can be effectively applied particularly to white LED applications, and the brightness of the white LED can be improved.
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äœã¯R-L-M-O-NïŒZç³»ã®é
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äœã§ãããããã§Zã¯è³ŠæŽ»å€ã§Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Euã奜ãŸãããRã¯ãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ããããããã®äžã§ã¯Y,Gd,Ybã奜ãŸãããLã¯Be,Mg,Ca,Sr,Baãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Ca,Sr,Baã奜ãŸãããMã¯C,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Siã奜ãŸããã
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äœã®å¥œãŸããçµæç¯å²ã¯ZãïŒãïŒïŒååïŒ
ãRãïŒãïŒïŒååïŒ
ãLãïŒãïŒïŒååïŒ
ãMãïŒãïŒïŒååïŒ
ã§ããããŸãé
žçŽ ãšçªçŽ ã®æ¯ã¯é
žçŽ ïŒã°ã©ã ååã«å¯ŸãçªçŽ ïŒïŒïŒãïŒïŒã°ã©ã ååã§ããã
The first phosphor of the present invention is an RLMON: Z-based oxynitride phosphor. Z is an activator selected from the group consisting of at least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb. At least one element. Of these, Eu is preferred. R is one or more elements selected from the group consisting of Sc, Y, La, Gd, and Yb. Among these, Y, Gd, and Yb are preferable. L is at least one element selected from the group consisting of Be, Mg, Ca, Sr, and Ba. Of these, Ca, Sr, and Ba are preferable. M is at least one element selected from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf. Of these, Si is preferred.
A preferable composition range of the phosphor is such that Z is 1 to 20 atomic%, R is 1 to 30 atomic%, L is 1 to 30 atomic%, and M is 1 to 30 atomic%. The ratio of oxygen to nitrogen is 0.1 to 10 gram atoms of nitrogen with respect to 1 gram atom of oxygen.
æ¬çºæã®ç¬¬ïŒã®èå
äœã¯D-L-M-O-NïŒZç³»ã®é
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äœã§ãããããã§Zã¯è³ŠæŽ»å€ã§Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Euã奜ãŸãããDã¯ãLi,Na,K,Rb,Csãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Liã奜ãŸãããLã¯Be,Mg,Ca,Sr,Baãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Ca,Sr,Baã奜ãŸãããMã¯C,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Siã奜ãŸããã
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äœã®å¥œãŸããçµæç¯å²ã¯ZãïŒãïŒïŒååïŒ
ãDãïŒãïŒïŒååïŒ
ãLãïŒãïŒïŒååïŒ
ãMãïŒãïŒïŒååïŒ
ã§ããããŸãé
žçŽ ãšçªçŽ ã®æ¯ã¯é
žçŽ ïŒã°ã©ã ååã«å¯ŸãçªçŽ ïŒïŒïŒãïŒïŒã°ã©ã ååã§ããã
The second phosphor of the present invention is a DLMON: Z-based oxynitride phosphor. Z is an activator selected from the group consisting of at least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb. At least one element. Of these, Eu is preferred. D is at least one element selected from the group consisting of Li, Na, K, Rb, and Cs. Of these, Li is preferred. L is at least one element selected from the group consisting of Be, Mg, Ca, Sr, and Ba. Of these, Ca, Sr, and Ba are preferable. M is at least one element selected from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf. Of these, Si is preferred.
The preferable composition range of the phosphor is 1 to 20 atomic%, Z is 1 to 30 atomic%, L is 1 to 30 atomic%, and M is 1 to 30 atomic%. The ratio of oxygen to nitrogen is 0.1 to 10 gram atoms of nitrogen with respect to 1 gram atom of oxygen.
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äœã§ãããããã§Zã¯è³ŠæŽ»å€ã§Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Euã奜ãŸãããDã¯ãLi,Na,K,Rb,Csãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Liã奜ãŸãããRã¯ãSc,Y,La,Gd,Ybãããªã矀ããéžã°ããïŒçš®ä»¥äžã®å
çŽ ã§ããããããã®äžã§ã¯Y,Gd,Ybã奜ãŸãããLã¯Be,Mg,Ca,Sr,Baãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
çŽ ã§ããããããã®äžã§ã¯Ca,Sr,Baã奜ãŸãããMã¯C,Si,Ge,Sn,Ti,Zr,Hfãããªã矀ããéžã°ããå°ãªããšãïŒçš®ã®å
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ãLãïŒãïŒïŒååïŒ
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The third phosphor of the present invention is a DRLMON: Z-based oxynitride phosphor. Z is an activator selected from the group consisting of at least one element selected from the group consisting of Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, and Sb. At least one element. Of these, Eu is preferred. D is at least one element selected from the group consisting of Li, Na, K, Rb, and Cs. Of these, Li is preferred. R is one or more elements selected from the group consisting of Sc, Y, La, Gd, and Yb. Among these, Y, Gd, and Yb are preferable. L is at least one element selected from the group consisting of Be, Mg, Ca, Sr, and Ba. Of these, Ca, Sr, and Ba are preferable. M is at least one element selected from the group consisting of C, Si, Ge, Sn, Ti, Zr, and Hf. Of these, Si is preferred.
The preferable composition range of the phosphor is 1 to 20 atomic%, Z is 1 to 30 atomic%, R is 1 to 30 atomic%, L is 1 to 30 atomic%, and M is 1 to 30 atomic%. The ratio of oxygen to nitrogen is 0.1 to 10 gram atoms of nitrogen with respect to 1 gram atom of oxygen.
The phosphor of the present invention is generally used as a powder, and the particle size (average particle size) is preferably 50 ÎŒm or less.
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žåç©ãçªåç©ã圢æããååç©ã®å°ãªããšãäžçš®ãšãCãæãã¯C以å€ã®Mã®äžããéžã°ããå
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žåç©ãçªåç©ã圢æããååç©ãšãçšããããããæ··åããç空ãããã¯éé
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ã奜ãŸãããååæã¯åºäœã§äœ¿çšããå Žåã¯ç²æ«ã«ããŠçšããããããŸãååç©ã氎溶液ã«ããŠã次ãã§æ²æ®¿ãããæ¿Ÿéã也ç¥ããŠçšããããšãã§ããã
The oxynitride phosphor of the present invention can be obtained as follows.
The RLMON: Z-based oxynitride phosphor is at least one element selected from the elements of Z described above as a raw material, an oxide, a nitride, or a compound that forms these oxides and nitrides by heating. At least one element selected from R elements, oxides, nitrides, or compounds that form these oxides and nitrides by heating, and elements selected from L, oxidation At least one of these oxides, nitrides or compounds that form nitrides by heating, and elements selected from C or M other than C, oxides, nitrides, or these oxides by heating, It can be obtained by using a compound that forms a nitride, mixing them, and firing at 900 to 1900 ° C. in a vacuum or non-oxidizing atmosphere. In the above, when an element other than C (carbon) is used as M, carbon may be mixed therewith. The mixing ratio of each element in the raw material mixture is preferably set so that the produced phosphor has the above-described composition. However, when carbon is used alone as M element, and when used together with Si or the like, the amount is preferably 0.1 to 20% by mass in the raw material mixture. Each raw material is used as a powder when used in a solid form. Alternatively, the compound can be used as an aqueous solution, then precipitated, filtered and dried.
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ã奜ãŸãããååæã¯åºäœã§äœ¿çšããå Žåã¯ç²æ«ã«ããŠçšããããããŸãååç©ã氎溶液ã«ããŠã次ãã§æ²æ®¿ãããæ¿Ÿéã也ç¥ããŠçšããããšãã§ããã
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The DRLMON: Z-based oxynitride phosphor of the present invention forms at least one element selected from among the elements of Z described above as a raw material, oxide, nitride, or these oxides and nitrides by heating. At least one compound selected from at least one element selected from the elements of D, oxides, nitrides, or at least one compound that forms these oxides and nitrides by heating, and elements of R At least one element selected from oxides, nitrides, or at least one of these oxides and compounds that form nitrides by heating, and elements selected from L, oxides, nitrides, or these by heating At least one of compounds that form oxides and nitrides, and elements selected from C or M other than C, oxides, nitrides, or compounds that form these oxides or nitrides by heating The reference can These were mixed, obtained by calcining at 900 to 1,900 ° C. in a vacuum or non-oxidizing atmosphere. In the above, when an element other than C (carbon) is used as M, carbon may be mixed therewith. The mixing ratio of each element in the raw material mixture is preferably set so that the produced phosphor has the above-described composition. However, when carbon is used alone as M element, and when used together with Si or the like, the amount is preferably 0.1 to 20% by mass in the raw material mixture. Each raw material is used as a powder when used in a solid form. Alternatively, the compound can be used as an aqueous solution, then precipitated, filtered and dried.
Since the phosphor of the present invention contains O and N, at least one oxide is necessary for the raw material mixture. In addition, it is necessary to use at least one nitride, or to use a single element or oxide and nitride it to contain nitrogen. In any case, when a single element or oxide is used, the atmosphere for firing the mixed raw material is set to a nitrogen-containing atmosphere, and the element is nitrided.
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Ce,Pr,Nd,Sm,Eu,Tb,Dy,Ho,Er,Tm,Cr,Mn,Pb,Sbã«ã€ããŠã¯ããããã®åäœéå±ãçªåç©ãé
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Next, each raw material used for production of the phosphor of the present invention will be described.
For Ce, Pr, Nd, Sm, Eu, Tb, Dy, Ho, Er, Tm, Cr, Mn, Pb, Sb, these single metals, nitrides, oxides, or heating (including nitrogen atmosphere) It is possible to select and use one or more of carbonates, hydroxides, oxalates, sulfates, nitrates, acetates and organometallic compounds containing these elements that form oxides and nitrides. Yes, two or more kinds of mixtures, composite oxides, solid solutions, mixed crystals and the like can also be used.
In the above, Eu will be taken up and described in more detail. As a raw material compound of Eu, a single metal, europium nitride, an oxide, or a compound that forms oxide or nitride by heating can be used. For example, one or more selected from europium oxide, europium carbonate, europium hydroxide, europium oxalate, europium sulfate, europium nitrate, europium acetate, trimethoxy europium, triethoxy europium, tripropoxy europium, tributoxy europium, etc. Two or more kinds of mixtures, composite oxides, solid solutions, mixed crystals and the like can also be used.
Sc,Y,La,Gd,Yb ã«ã€ããŠã¯ããããã®åäœéå±ãçªåç©ãé
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For Sc, Y, La, Gd, and Yb, these simple metals, nitrides, oxides, or carbonates, hydroxides, oxalates, oxides and nitrides formed by heating (including nitrogen atmosphere), It is possible to select one or more from sulfates, nitrates, acetates and organometallic compounds containing these elements, etc., and mixtures of two or more, complex oxides, solid solutions, mixed crystals, etc. Can be used.
In the above, Y is taken up and explained in more detail. As a raw material compound for Y, a single metal, yttrium nitride, an oxide, or a compound that forms an oxide or nitride by heating can be used. For example, use one or more selected from yttrium oxide, yttrium carbonate, yttrium hydroxide, yttrium oxalate, yttrium sulfate, yttrium nitrate, yttrium acetate, trimethoxy yttrium, triethoxy yttrium, tripropoxy yttrium, tributoxy yttrium, etc. Two or more kinds of mixtures, composite oxides, solid solutions, mixed crystals and the like can also be used.
BeïŒMgïŒCaïŒSrïŒBaæºã®åæã¯BeïŒMgïŒCaïŒSrïŒBaãããªã矀ããéžã°ããäžçš®ä»¥äžã®åäœéå±ãé žåããªãªãŠã ãé žåãã°ãã·ãŠã ãé žåã¹ããã³ããŠã ãé žåããªãŠã é žåç©ãããã¯ãçªåããªãªãŠã ãçªåãã°ãã·ãŠã ãçªåã¹ããã³ããŠã ãçªåããªãŠã ãæãã¯BeïŒMgïŒCaïŒSrïŒBaãããªã矀ããéžã°ããäžçš®ä»¥äžã®ååç©ã§ãã£ãŠå ç±ã«ããé žåç©ãçªåç©ã圢æãããã®ã䜿çšããããšãã§ãããå ·äœçã«ã¯çé žããªãªãŠã ãçé žãã°ãã·ãŠã ãçé žã¹ããã³ããŠã ãçé žããªãŠã ãæ°Žé žåããªãªãŠã ãæ°Žé žåãã°ãã·ãŠã ãæ°Žé žåã¹ããã³ããŠã ãæ°Žé žåããªãŠã ãèé žããªãªãŠã ãèé žãã°ãã·ãŠã ãèé žã¹ããã³ããŠã ãèé žããªãŠã ãç¡«é žããªãªãŠã ãç¡«é žãã°ãã·ãŠã ãç¡«é žã«ã«ã·ãŠã ãç¡«é žã¹ããã³ããŠã ãç¡«é žããªãŠã ãç¡é žããªãªãŠã ãç¡é žãã°ãã·ãŠã ãç¡é žã«ã«ã·ãŠã ãç¡é žã¹ããã³ããŠã ãç¡é žããªãŠã ãé ¢é žããªãªãŠã ãé ¢é žãã°ãã·ãŠã ãé ¢é žã«ã«ã·ãŠã ãé ¢é žã¹ããã³ããŠã ãé ¢é žããªãŠã ããžã¡ããã·ããªãªãŠã ããžã¡ããã·ãã°ãã·ãŠã ããžã¡ããã·ã«ã«ã·ãŠã ããžã¡ããã·ã¹ããã³ããŠã ããžã¡ããã·ããªãŠã ããžãšããã·ããªãªãŠã ããžãšããã·ãã°ãã·ãŠã ããžãšããã·ã«ã«ã·ãŠã ããžãšããã·ã¹ããã³ããŠã ããžãšããã·ããªãŠã ããžããããã·ããªãªãŠã ããžããããã·ãã°ãã·ãŠã ããžããããã·ã«ã«ã·ãŠã ããžããããã·ã¹ããã³ããŠã ããžããããã·ããªãŠã ããžãããã·ããªãªãŠã ããžãããã·ãã°ãã·ãŠã ããžãããã·ã«ã«ã·ãŠã ããžãããã·ã¹ããã³ããŠã ããžãããã·ããªãŠã ããã¹ïŒãžãããã€ã«ã¡ã¿ããïŒããªãªãŠã ããã¹ïŒãžãããã€ã«ã¡ã¿ããïŒãã°ãã·ãŠã ããã¹ïŒãžãããã€ã«ã¡ã¿ããïŒã«ã«ã·ãŠã ããã¹ïŒãžãããã€ã«ã¡ã¿ããïŒã¹ããã³ããŠã ããã¹ïŒãžãããã€ã«ã¡ã¿ããïŒããªãŠã ããªã©ããïŒçš®ä»¥äžãéžæããŠäœ¿çšããããšãå¯èœã§ãããïŒçš®ä»¥äžã®æ··åç©ãè€åé žåç©ãåºæº¶äœãæ··æ¶ãªã©ã䜿çšã§ããã The source material for Be, Mg, Ca, Sr, and Ba is one or more elemental metals selected from the group consisting of Be, Mg, Ca, Sr, and Ba, beryllium oxide, magnesium oxide, strontium oxide, barium oxide, or nitride It is possible to use one or more compounds selected from the group consisting of beryllium, magnesium nitride, strontium nitride, barium nitride, or Be, Mg, Ca, Sr, and Ba, which form oxides and nitrides by heating. it can. Specifically, beryllium carbonate, magnesium carbonate, strontium carbonate, barium carbonate, beryllium hydroxide, magnesium hydroxide, strontium hydroxide, barium hydroxide, beryllium oxalate, magnesium oxalate, strontium oxalate, barium oxalate, beryllium sulfate, magnesium sulfate, Calcium sulfate, strontium sulfate, barium sulfate, beryllium nitrate, magnesium nitrate, calcium nitrate, strontium nitrate, barium nitrate, beryllium acetate, magnesium acetate, calcium acetate, strontium acetate, barium acetate, dimethoxyberyllium, dimethoxymagnesium, dimethoxycalcium, dimethoxystrontium , Dimethoxybarium, diethoxyberyllium, diethoxymagnesium, diethoxycalcium, diethoxy Trontium, diethoxybarium, dipropoxyberyllium, dipropoxymagnesium, dipropoxycalcium, dipropoxystrontium, dipropoxybarium, dibutoxyberyllium, dibutoxymagnesium, dibutoxycalcium, dibutoxystrontium, dibutoxybarium, bis (dipi Baroylmethanato) Beryllium, bis (dipivaloylmethanato) magnesium, bis (dipivaloylmethanato) calcium, bis (dipivaloylmethanato) strontium, bis (dipivaloylmethanato) barium, etc. The above can be selected and used, and two or more kinds of mixtures, composite oxides, solid solutions, mixed crystals and the like can also be used.
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žå¡©è¥ããã¯æ°Žé
žåç©ã§ãããç¹ã«å¥œãŸãããã®ã¯ãçé
žå¡©ã§ããã
Si,Ge,Sn,Ti,Zr,Hfã®åæååç©ãšããŠã¯ãåäœéå±ãçªåç©ãé
žåç©ãæãã¯å ç±ã«ããçªåç©ãé
žåç©ã圢æããçé
žå¡©ãæ°Žé
žåç©ãèé
žå¡©ãç¡«é
žå¡©ãç¡é
žå¡©ãé
¢é
žå¡©ãSi,Ge,Sn,Ti,Zr,Hfãå«æããææ©éå±ååç©ãªã©ããïŒçš®ä»¥äžãéžæããŠäœ¿çšããããšãå¯èœã§ãããïŒçš®ä»¥äžã®æ··åç©ãè€åé
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CãšããŠã¯ãç¡å®åœ¢ççŽ ãé»éçã䜿çšããããšãå¯èœã§ããã
Preferred among these compounds are carbonates or hydroxides. Particularly preferred is carbonate.
As raw materials of Si, Ge, Sn, Ti, Zr, Hf, simple metals, nitrides, oxides, or nitrides by heating, carbonates that form oxides, hydroxides, oxalates, sulfates, It is possible to select one or more types from nitrates, acetates, organometallic compounds containing Si, Ge, Sn, Ti, Zr, Hf, etc., and mixtures of two or more types, complex oxides, solid solutions Also, mixed crystals can be used.
As C, amorphous carbon, graphite or the like can be used.
äžèšã«ãããSiã«ã€ããŠããã«è©³ãã説æããã
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žåçªçŽ ãçªåçªçŽ ãé
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é
žåçªçŽ ã®åæååç©ãšããŠã¯ãé
žåçªçŽ æãã¯å ç±ã«ããé
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žåçªçŽ ãäžé
žåçªçŽ ãããã©ã¡ããã·ã·ã©ã³ãããã©ãšããã·ã·ã©ã³ãããã©ããããã·ã·ã©ã³ãããã©ãããã·ã·ã©ã³ãããªã¹ïŒãžã¡ãã«ã¢ããïŒã·ã©ã³ããªã©ããïŒçš®ä»¥äžãéžæããŠäœ¿çšããããšãå¯èœã§ãããïŒçš®ä»¥äžã®æ··åç©ãåºæº¶äœãæ··æ¶ãªã©ã䜿çšã§ããã
Si in the above will be described in more detail.
As a raw material compound of Si, silicon oxide, silicon nitride, silicon oxynitride, or the like can be used.
As a raw material compound of silicon oxide, silicon oxide or a compound that forms silicon oxide by heating can be used. For example, one or more selected from silicon dioxide, silicon monoxide, tetramethoxysilane, tetraethoxysilane, tetrapropoxysilane, tetrabutoxysilane, tris (dimethylamino) silane, and the like can be used. Mixtures, solid solutions, mixed crystals, etc. of seeds or more can also be used.
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žåçªçŽ ãäžé
žåçªçŽ ãããã©ã¡ããã·ã·ã©ã³ãããã©ãšããã·ã·ã©ã³ãããã©ããããã·ã·ã©ã³ãããã©ãããã·ã·ã©ã³ãããªã¹ïŒãžã¡ãã«ã¢ããïŒã·ã©ã³ãããéžã°ããäžçš®ä»¥äžã®ååç©ã«ãå¿
èŠã«ããççŽ è¥ããã¯å ç±ã«ããççŽ ã圢æããååç©ãšãæ··åããçªçŽ è¥ããã¯çªçŽ å«æéé
žåæ§é°å²æ°äžã§å ç±ããŠããåæ§ã®çµæãåŸãããšãåºæ¥ãããããã®åæã®ãã¡ãåºäœã§ãããã®ã¯ãç²æ«ç¶æ
ã§ããããšã奜ãŸãããç²åºŠã¯ç¹ã«éå®ãããªããã埮现åæã®æ¹ãåå¿æ§ã«åªããããã奜ãŸãããçŽåºŠã¯ã90ïŒ
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ãŸããäžèšããååç©ã®ãã¡ãå ç±ã«ããé
žåç©ã圢æããååç©ãšãççŽ ãããã¯éç±ã«ããççŽ ã圢æããååç©ãšãå
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As the silicon nitride raw material compound, silicon nitride or a compound that forms silicon nitride by heating can be used. For example, it is possible to use one or more selected from silicon diimide, polysilazane and the like. Furthermore, one or more compounds selected from silicon, silicon dioxide, silicon monoxide, tetramethoxysilane, tetraethoxysilane, tetrapropoxysilane, tetrabutoxysilane, and tris (dimethylamino) silane are added to carbon or carbon by heating as necessary. A similar result can be obtained by mixing with a compound that forms, and heating in nitrogen or a nitrogen-containing non-oxidizing atmosphere. Among these raw materials, those that are solid are preferably in a powder state. The particle size is not particularly limited, but a fine raw material is preferable because it is excellent in reactivity. The purity is preferably 90% or more.
Of the above-mentioned compounds, a compound that forms an oxide by heating and a compound that forms carbon by heating or carbon coexist, and is fired in a nitrogen-containing non-oxidizing atmosphere, whereby nitride or oxynitride To form a raw material compound.
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žåç©ã圢æããååç©åã³å ç±ã«ããçªåç©ã圢æããååç©ãšãççŽ ãããã¯éç±ã«ããççŽ ã圢æããååç©ãšãå
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Li,Na,K,Rb,Csæºã®åæãšããŠã¯ããããã®åäœå
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Further, a compound that forms an oxide by heating, a compound that forms an oxide by heating, a compound that forms a nitride by heating, and a compound that forms carbon by heating or overheating coexist with a nitrogen-containing non-oxidizing atmosphere. The target oxynitride phosphor can be formed by firing in the medium.
As raw materials for the Li, Na, K, Rb, and Cs sources, these simple elements, oxides, nitrides, or compounds that can be converted into oxides and nitrides by heating are used. For example, inorganic compounds such as hydroxide, carbonate, chloride, nitrate, sulfate, and other organic compounds containing these elements can also be used. Of these, carbonate is preferred.
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The production method of the oxynitride phosphor of the present invention is not particularly limited, and any of a solid phase method, a liquid phase method, and a gas phase method can be adopted. A method can be exemplified.
First, raw material compounds are weighed and mixed in a desired ratio. For the mixing, a ball mill can be used. When performing ball mill mixing, dry mixing is possible, but wet mixing using ethanol, acetone, water, or the like can also be performed. In order to increase the reactivity of the raw material powder, wet mixing is desirable. When performing wet mixing, after drying the obtained mixed slurry, it is crushed as needed.
Here, if necessary, the raw material compound may be mixed with a flux. As the flux, alkali metal halides or alkaline earth metal halides can be used. For example, the flux is added in the range of 0.01 to 1 part by weight with respect to 100 parts by weight of the phosphor raw material.
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This raw material mixture is filled in a crucible made of alumina, calcia, magnesia, graphite, boron nitride or the like, and fired at 900 to 1900 ° C. for several hours in a vacuum or non-oxidizing atmosphere. If necessary, non-oxidizing atmosphere pressurization may be performed. Here, the non-oxidizing atmosphere is nitrogen, nitrogen-hydrogen, argon-hydrogen, ammonia, argon, nitrogen-cyan gas, argon-cyan gas, nitrogen-carbon monoxide, argon-carbon monoxide, or the like.
In the phosphor of the present invention, the activator Z, particularly europium, emits good light when it is positively divalent. Since europium oxide used as a raw material is trivalent, it must be reduced in the firing process. The ratio of divalent and trivalent is better as the divalent is higher, and the ratio of divalent to the total europium is preferably 50% or more. More preferably, it is 80% or more. In the phosphor of the present invention, europium is added by replacing the site of the divalent alkaline earth metal element. Therefore, if the trivalent europium remains, the balance of charge is lost and the emission intensity is reduced.
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In addition, when carbon or a carbon-containing compound is allowed to coexist during firing of the raw material mixture, the reduction of europium oxide proceeds rapidly. The carbon or carbon-containing compound used here may be amorphous carbon, graphite, silicon carbide or the like, and is not particularly limited, but is preferably amorphous carbon, graphite or the like. Carbon black, graphite powder, activated carbon, silicon carbide powder, and the like, as well as these molded products, sintered bodies, and the like can be exemplified, but all can obtain the same effect. As an aspect of coexistence, when used as a crucible made of carbon or a carbon-containing compound, when placed inside or outside a crucible made of a material other than carbon or a carbon-containing compound, a heating element or a heat insulator made of carbon or a carbon-containing compound In the case of using as, when carbon or a carbon-containing compound is mixed in the raw material mixture, etc., the same effect can be obtained by adopting any arrangement method. The coexisting carbon or carbon-containing compound is, for example, about equimolar to the europium oxide in the raw material mixture when powdered carbon is contained in the raw material mixture and calcined in a nitrogen atmosphere.
After cooling, if necessary, disperse and pulverize with a ball mill, etc., and further with water washing as necessary, and obtain the phosphor of the present invention through steps such as solid-liquid separation, drying, crushing, and classification. be able to.
Since the phosphor of the present invention is efficiently excited by ultraviolet rays or visible light of 250 to 500 nm, it can be effectively applied to white LED applications using ultraviolet LEDs or blue LEDs.
æ¬çºæã®å¥œãŸããå®æœæ æ§ã§ããèå äœãšïŒïŒïŒïœïœããïŒïŒïŒïœïœã®æ³¢é·åã«çºå ããåå°äœçºå çŽ åãçµã¿åãããŠçºå è£ çœ®ãæ§æããããšãå¯èœã§ããããã®å Žåã®çºå çŽ åãšããŠã¯ZnSeãGaNãªã©çš®ã ã®åå°äœãæãããããçºå çŽ åã¯ãçºå ã¹ãã¯ãã«ãïŒïŒïŒïœïœããïŒïŒïŒïœïœã«çºå å¯èœãªãã®ã§ããã°ééãªã䜿çšå¯èœã§ããããå¹çã®ç¹ããã¯çªåã¬ãªãŠã ç³»ååç©åå°äœã奜ãŸããçšãããããçºå çŽ åã¯ïŒïŒ¯ïŒ£ïŒ¶ïŒ€æ³ãæ³çã«ããåºæ¿äžã«çªåç©ç³»ååç©åå°äœã圢æãããŠåŸããã奜ãŸããã¯InαAlβGa1-α-βNïŒäœããïŒâŠÎ±ãïŒâŠÎ²ãαïŒÎ²âŠïŒïŒãçºå å±€ãšããŠåœ¢æããããåå°äœã®æ§é ãšããŠã¯ãïŒïŒ©ïŒ³æ¥åãæ¥åãïœïœæ¥åãªã©ãæãããã¢æ§é ããããæ§é ãããã¯ããã«ãããæ§é ã®ãã®ãæãããããåå°äœå±€ã®ææããã®æ··æ¶åºŠã«ãã£ãŠçºå æ³¢é·ãçš®ã éžæããããšãã§ããããŸããåå°äœæŽ»æ§å±€ãéåå¹æãçããèèã«åœ¢æãããåäžéåäºæžæ§é ãå€ééåäºæžæ§é ãšããããšãã§ããã It is also possible to constitute a light emitting device by combining a phosphor that is a preferred embodiment of the present invention and a semiconductor light emitting element that emits light in a wavelength range of 250 nm to 500 nm. In this case, examples of the light emitting element include various semiconductors such as ZnSe and GaN. The light-emitting element can be used without limitation as long as the emission spectrum can emit light from 250 nm to 500 nm, but a gallium nitride-based compound semiconductor is preferably used from the viewpoint of efficiency. The light emitting element is obtained by forming a nitride compound semiconductor on a substrate by MOCVD method, HVPE method or the like, preferably In α Al β Ga 1-α-β N (where 0 ⊠α, 0 ⊠β, α + β ⊠1) is formed as the light emitting layer. Examples of the semiconductor structure include a homostructure, a heterostructure, or a double heterostructure having a MIS junction, a PIN junction, a pn junction, or the like. Various emission wavelengths can be selected depending on the material of the semiconductor layer and the degree of mixed crystal. In addition, a single quantum well structure or a multiple quantum well structure in which the semiconductor active layer is formed in a thin film in which a quantum effect is generated can be used.
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The phosphor layer provided on the light emitting element may be arranged by laminating at least one or more kinds of phosphors as a single layer or a plurality of layers, or a mixture of a plurality of phosphors in a single layer. You may do it. As a form of providing the phosphor layer on the light emitting element, a form in which the phosphor is mixed with a coating member that covers the surface of the light emitting element, a form in which the phosphor is mixed with the mold member, or a fluorescent substance is applied to the covering on the mold member. The form which mixes a body, Furthermore, the form which arrange | positions the translucent plate which mixed the fluorescent substance in the light emission side front of an LED lamp etc. are mentioned.
The phosphor may be added with at least one kind of phosphor to a mold member on the light emitting element. Further, one or more phosphor layers of the above phosphors may be provided outside the light emitting diode. As a form provided on the outside of the light emitting diode, a form in which the phosphor is applied in a layer form on the outer surface of the mold member of the light emitting diode, or a molded body in which the phosphor is dispersed in rubber, resin, elastomer, low melting point glass or the like (for example, (Cap shape) and the form which coat | covers this to LED, or the form which processes the said molded object into flat form, and arranges this in front of LED etc. are mentioned.
Also for mold members. A diffusing agent such as titanium oxide, titanium nitride, tantalum nitride, aluminum oxide, silicon oxide, or barium titanate can also be contained.
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žåçªçŽ ç²æ«ã13.00ïœãšãçªåçªçŽ ç²æ«ã30.35ïœãšãçé
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Examples of the present invention will be described below, but the present invention is not limited to specific examples. In the following examples, the emission spectrum was measured using FP-6500 manufactured by JASCO Corporation.
[Example 1] As a phosphor constituent material, 3.80 g of europium oxide powder, 13.00 g of silicon oxide powder, 30.35 g of silicon nitride powder, 44.73 g of strontium carbonate powder, and 6.11 g of yttrium oxide powder Then, 2.00 g of lithium carbonate powder was accurately weighed and uniformly mixed by a wet method using ethanol using a ball mill, and the resulting slurry was dried and crushed to obtain a raw material mixture. Next, the obtained raw material mixture was put in a graphite crucible, placed in an alumina furnace core tube, and fired at a temperature of 1300 ° C. for 6 hours in a nitrogen stream. The obtained fired product was finely pulverized and classified by a ball mill to obtain a phosphor having an average particle size of 4.5 Όm. When the phosphor was made to emit light under 450 nm excitation, yellow-green light emission was observed.
å®æœäŸïŒïŒœèå äœæ§æåæãšããŠãé žåãŠãŒãããŠã ç²æ«ã4.05ïœãšãé žåçªçŽ ç²æ«ã13.85ïœãšãçªåçªçŽ ç²æ«ã32.33ïœãšãçé žã¹ããã³ããŠã ç²æ«ã47.64ïœãšãçé žãªããŠã ç²æ«ã2.13gãšãæ£ç¢ºã«ç§€éãããããããŒã«ãã«ã䜿çšããšã¿ããŒã«ãçšãã湿åŒæ³ã«ããåäžã«æ··åããåŸãããã¹ã©ãªãŒã也ç¥ã解ç ããŠåææ··åäœãšããã次ã«ãåŸãããåææ··åäœããé»é補å©å ã«å ¥ãã¢ã«ãã補çå¿ç®¡äžã«é 眮ããçªçŽ æ°æµäžïŒïŒïŒïŒâã®æž©åºŠã§ïŒæéçŒæãããåŸãããçŒæç©ãããŒã«ãã«ã«ãã现ããç²ç ã»åçŽããå¹³åç²åŸïŒïŒïŒÎŒïœã®èå äœãšãããåèå äœã450ïœïœå±èµ·äžã§çºå ããããšãããé»ç·è²çºå ãèªããããã [Example 2] 4.05 g of europium oxide powder, 13.85 g of silicon oxide powder, 32.33 g of silicon nitride powder, 47.64 g of strontium carbonate powder, 2.13 g of lithium carbonate powder as phosphor constituting materials Was accurately weighed and uniformly mixed by a wet method using ethanol using a ball mill, and the resulting slurry was dried and crushed to obtain a raw material mixture. Next, the obtained raw material mixture was put in a graphite crucible, placed in an alumina furnace core tube, and fired at a temperature of 1300 ° C. for 6 hours in a nitrogen stream. The obtained fired product was finely pulverized and classified by a ball mill to obtain a phosphor having an average particle size of 4.3 ÎŒm. When the phosphor was made to emit light under 450 nm excitation, yellow-green light emission was observed.
å®æœäŸïŒïŒœèå äœæ§æåæãšããŠãé žåãŠãŒãããŠã ç²æ«ã3.89ïœãšãé žåçªçŽ ç²æ«ã13.26ïœãšãçªåçªçŽ ç²æ«ã30.98ïœãšãçé žã¹ããã³ããŠã ç²æ«ã45.64ïœãšãé žåã€ãããªãŠã ç²æ«ã6.23gãšãæ£ç¢ºã«ç§€éãããããããŒã«ãã«ã䜿çšããšã¿ããŒã«ãçšãã湿åŒæ³ã«ããåäžã«æ··åããåŸãããã¹ã©ãªãŒã也ç¥ã解ç ããŠåææ··åäœãšããã次ã«ãåŸãããåææ··åäœããé»é補å©å ã«å ¥ãã¢ã«ãã補çå¿ç®¡äžã«é 眮ããçªçŽ æ°æµäžïŒïŒïŒïŒâã®æž©åºŠã§ïŒæéçŒæãããåŸãããçŒæç©ãããŒã«ãã«ã«ãã现ããç²ç ã»åçŽããå¹³åç²åŸïŒïŒïŒÎŒïœã®èå äœãšãããåèå äœã450ïœïœå±èµ·äžã§çºå ããããšãããé»ç·è²çºå ãèªããããã [Example 3] As a phosphor constituting material, 3.89 g of europium oxide powder, 13.26 g of silicon oxide powder, 30.98 g of silicon nitride powder, 45.64 g of strontium carbonate powder, and 6.23 g of yttrium oxide powder Was accurately weighed and uniformly mixed by a wet method using ethanol using a ball mill, and the resulting slurry was dried and crushed to obtain a raw material mixture. Next, the obtained raw material mixture was put in a graphite crucible, placed in an alumina furnace core tube, and fired at a temperature of 1400 ° C. for 6 hours in a nitrogen stream. The obtained fired product was finely pulverized and classified by a ball mill to obtain a phosphor having an average particle size of 4.1 ÎŒm. When the phosphor was made to emit light under 450 nm excitation, yellow-green light emission was observed.
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The phosphor of the present invention can be combined with a blue light emitting diode or the like to produce white light, and can be used as an illumination light source or a display light source.
Claims (8)
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| Application Number | Priority Date | Filing Date | Title |
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| JP2005172282A JP2006348070A (en) | 2005-06-13 | 2005-06-13 | Oxynitride-based phosphor and method for producing the same |
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| JP2005172282A JP2006348070A (en) | 2005-06-13 | 2005-06-13 | Oxynitride-based phosphor and method for producing the same |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2008126500A1 (en) * | 2007-03-28 | 2008-10-23 | Hiroshima University | M-c-n-o fluorescent substance |
| JP2008266385A (en) * | 2007-04-17 | 2008-11-06 | Showa Denko Kk | Phosphor, method for manufacturing the same, and light emitting device using the same |
| JP2009079069A (en) * | 2007-09-25 | 2009-04-16 | Nichia Corp | Carbonitride phosphor, light-emitting device using the same, and method for producing carbonitride phosphor |
| KR101528104B1 (en) * | 2014-06-11 | 2015-06-11 | 죌ìíì¬ íšì± | Oxynitride phosphor of improved reliability, method for manufacturing thereof, and white emitting device comprising the same |
-
2005
- 2005-06-13 JP JP2005172282A patent/JP2006348070A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2008126500A1 (en) * | 2007-03-28 | 2008-10-23 | Hiroshima University | M-c-n-o fluorescent substance |
| US8668843B2 (en) | 2007-03-28 | 2014-03-11 | Hiroshima University | M-C-N-O based phosphor |
| JP2008266385A (en) * | 2007-04-17 | 2008-11-06 | Showa Denko Kk | Phosphor, method for manufacturing the same, and light emitting device using the same |
| JP2009079069A (en) * | 2007-09-25 | 2009-04-16 | Nichia Corp | Carbonitride phosphor, light-emitting device using the same, and method for producing carbonitride phosphor |
| KR101528104B1 (en) * | 2014-06-11 | 2015-06-11 | 죌ìíì¬ íšì± | Oxynitride phosphor of improved reliability, method for manufacturing thereof, and white emitting device comprising the same |
| WO2015190688A1 (en) * | 2014-06-11 | 2015-12-17 | 죌ìíì¬ íšì± | Oxynitride phosphor with improved reliability, method for preparing same, and white light emitting element comprising same |
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