TW200904946A - Green light-emitting fluorescent substance, method of manufacturing the same and light-emitting device using the same - Google Patents
Green light-emitting fluorescent substance, method of manufacturing the same and light-emitting device using the same Download PDFInfo
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- TW200904946A TW200904946A TW097122124A TW97122124A TW200904946A TW 200904946 A TW200904946 A TW 200904946A TW 097122124 A TW097122124 A TW 097122124A TW 97122124 A TW97122124 A TW 97122124A TW 200904946 A TW200904946 A TW 200904946A
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- green
- metal
- emitting
- light
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- YNKVVRHAQCDJQM-UHFFFAOYSA-P diazanium dinitrate Chemical compound [NH4+].[NH4+].[O-][N+]([O-])=O.[O-][N+]([O-])=O YNKVVRHAQCDJQM-UHFFFAOYSA-P 0.000 description 1
- TYIXMATWDRGMPF-UHFFFAOYSA-N dibismuth;oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Bi+3].[Bi+3] TYIXMATWDRGMPF-UHFFFAOYSA-N 0.000 description 1
- BEQZMQXCOWIHRY-UHFFFAOYSA-H dibismuth;trisulfate Chemical compound [Bi+3].[Bi+3].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O BEQZMQXCOWIHRY-UHFFFAOYSA-H 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 238000007580 dry-mixing Methods 0.000 description 1
- 229910003440 dysprosium oxide Inorganic materials 0.000 description 1
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(iii) oxide Chemical compound O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 description 1
- 238000004945 emulsification Methods 0.000 description 1
- 238000011049 filling Methods 0.000 description 1
- 150000002222 fluorine compounds Chemical class 0.000 description 1
- MEANOSLIBWSCIT-UHFFFAOYSA-K gadolinium trichloride Chemical compound Cl[Gd](Cl)Cl MEANOSLIBWSCIT-UHFFFAOYSA-K 0.000 description 1
- 229940119177 germanium dioxide Drugs 0.000 description 1
- BIXHRBFZLLFBFL-UHFFFAOYSA-N germanium nitride Chemical compound N#[Ge]N([Ge]#N)[Ge]#N BIXHRBFZLLFBFL-UHFFFAOYSA-N 0.000 description 1
- 229910052736 halogen Inorganic materials 0.000 description 1
- 125000005843 halogen group Chemical group 0.000 description 1
- 150000002367 halogens Chemical class 0.000 description 1
- LNEPOXFFQSENCJ-UHFFFAOYSA-N haloperidol Chemical compound C1CC(O)(C=2C=CC(Cl)=CC=2)CCN1CCCC(=O)C1=CC=C(F)C=C1 LNEPOXFFQSENCJ-UHFFFAOYSA-N 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 description 1
- OWCYYNSBGXMRQN-UHFFFAOYSA-N holmium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Ho+3].[Ho+3] OWCYYNSBGXMRQN-UHFFFAOYSA-N 0.000 description 1
- BDAGIHXWWSANSR-NJFSPNSNSA-N hydroxyformaldehyde Chemical compound O[14CH]=O BDAGIHXWWSANSR-NJFSPNSNSA-N 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- FYDKNKUEBJQCCN-UHFFFAOYSA-N lanthanum(3+);trinitrate Chemical compound [La+3].[O-][N+]([O-])=O.[O-][N+]([O-])=O.[O-][N+]([O-])=O FYDKNKUEBJQCCN-UHFFFAOYSA-N 0.000 description 1
- 229910001386 lithium phosphate Inorganic materials 0.000 description 1
- 229910003443 lutetium oxide Inorganic materials 0.000 description 1
- OTCKOJUMXQWKQG-UHFFFAOYSA-L magnesium bromide Chemical compound [Mg+2].[Br-].[Br-] OTCKOJUMXQWKQG-UHFFFAOYSA-L 0.000 description 1
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 1
- 239000001095 magnesium carbonate Substances 0.000 description 1
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
- 235000019341 magnesium sulphate Nutrition 0.000 description 1
- 239000011656 manganese carbonate Substances 0.000 description 1
- 235000006748 manganese carbonate Nutrition 0.000 description 1
- 229940093474 manganese carbonate Drugs 0.000 description 1
- 239000011565 manganese chloride Substances 0.000 description 1
- 235000002867 manganese chloride Nutrition 0.000 description 1
- 229940099607 manganese chloride Drugs 0.000 description 1
- 229940099596 manganese sulfate Drugs 0.000 description 1
- 239000011702 manganese sulphate Substances 0.000 description 1
- 235000007079 manganese sulphate Nutrition 0.000 description 1
- MIVBAHRSNUNMPP-UHFFFAOYSA-N manganese(2+);dinitrate Chemical compound [Mn+2].[O-][N+]([O-])=O.[O-][N+]([O-])=O MIVBAHRSNUNMPP-UHFFFAOYSA-N 0.000 description 1
- 229910000016 manganese(II) carbonate Inorganic materials 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
- XMWCXZJXESXBBY-UHFFFAOYSA-L manganese(ii) carbonate Chemical compound [Mn+2].[O-]C([O-])=O XMWCXZJXESXBBY-UHFFFAOYSA-L 0.000 description 1
- 238000001819 mass spectrum Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910001507 metal halide Inorganic materials 0.000 description 1
- 150000005309 metal halides Chemical class 0.000 description 1
- ATINCSYRHURBSP-UHFFFAOYSA-K neodymium(iii) chloride Chemical compound Cl[Nd](Cl)Cl ATINCSYRHURBSP-UHFFFAOYSA-K 0.000 description 1
- 229910000484 niobium oxide Inorganic materials 0.000 description 1
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- IHUHXSNGMLUYES-UHFFFAOYSA-J osmium(iv) chloride Chemical compound Cl[Os](Cl)(Cl)Cl IHUHXSNGMLUYES-UHFFFAOYSA-J 0.000 description 1
- MPARYNQUYZOBJM-UHFFFAOYSA-N oxo(oxolutetiooxy)lutetium Chemical compound O=[Lu]O[Lu]=O MPARYNQUYZOBJM-UHFFFAOYSA-N 0.000 description 1
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 1
- MMKQUGHLEMYQSG-UHFFFAOYSA-N oxygen(2-);praseodymium(3+) Chemical compound [O-2].[O-2].[O-2].[Pr+3].[Pr+3] MMKQUGHLEMYQSG-UHFFFAOYSA-N 0.000 description 1
- UZLYXNNZYFBAQO-UHFFFAOYSA-N oxygen(2-);ytterbium(3+) Chemical compound [O-2].[O-2].[O-2].[Yb+3].[Yb+3] UZLYXNNZYFBAQO-UHFFFAOYSA-N 0.000 description 1
- RVTZCBVAJQQJTK-UHFFFAOYSA-N oxygen(2-);zirconium(4+) Chemical compound [O-2].[O-2].[Zr+4] RVTZCBVAJQQJTK-UHFFFAOYSA-N 0.000 description 1
- VLTRZXGMWDSKGL-UHFFFAOYSA-N perchloric acid Chemical class OCl(=O)(=O)=O VLTRZXGMWDSKGL-UHFFFAOYSA-N 0.000 description 1
- 150000002978 peroxides Chemical class 0.000 description 1
- 229920005678 polyethylene based resin Polymers 0.000 description 1
- 229920005990 polystyrene resin Polymers 0.000 description 1
- 229910000105 potassium hydride Inorganic materials 0.000 description 1
- 229910003447 praseodymium oxide Inorganic materials 0.000 description 1
- LHBNLZDGIPPZLL-UHFFFAOYSA-K praseodymium(iii) chloride Chemical compound Cl[Pr](Cl)Cl LHBNLZDGIPPZLL-UHFFFAOYSA-K 0.000 description 1
- 229910052761 rare earth metal Inorganic materials 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- BHXBZLPMVFUQBQ-UHFFFAOYSA-K samarium(iii) chloride Chemical compound Cl[Sm](Cl)Cl BHXBZLPMVFUQBQ-UHFFFAOYSA-K 0.000 description 1
- 239000004576 sand Substances 0.000 description 1
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 229910000029 sodium carbonate Inorganic materials 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 230000003595 spectral effect Effects 0.000 description 1
- YJPVTCSBVRMESK-UHFFFAOYSA-L strontium bromide Chemical compound [Br-].[Br-].[Sr+2] YJPVTCSBVRMESK-UHFFFAOYSA-L 0.000 description 1
- 229910001625 strontium bromide Inorganic materials 0.000 description 1
- 229940074155 strontium bromide Drugs 0.000 description 1
- LSNNMFCWUKXFEE-UHFFFAOYSA-L sulfite Chemical class [O-]S([O-])=O LSNNMFCWUKXFEE-UHFFFAOYSA-L 0.000 description 1
- 150000003467 sulfuric acid derivatives Chemical class 0.000 description 1
- OEIMLTQPLAGXMX-UHFFFAOYSA-I tantalum(v) chloride Chemical compound Cl[Ta](Cl)(Cl)(Cl)Cl OEIMLTQPLAGXMX-UHFFFAOYSA-I 0.000 description 1
- 229910003451 terbium oxide Inorganic materials 0.000 description 1
- GFISHBQNVWAVFU-UHFFFAOYSA-K terbium(iii) chloride Chemical compound Cl[Tb](Cl)Cl GFISHBQNVWAVFU-UHFFFAOYSA-K 0.000 description 1
- SCRZPWWVSXWCMC-UHFFFAOYSA-N terbium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[Tb+3].[Tb+3] SCRZPWWVSXWCMC-UHFFFAOYSA-N 0.000 description 1
- 229920002803 thermoplastic polyurethane Polymers 0.000 description 1
- 150000003606 tin compounds Chemical class 0.000 description 1
- FAKFSJNVVCGEEI-UHFFFAOYSA-J tin(4+);disulfate Chemical compound [Sn+4].[O-]S([O-])(=O)=O.[O-]S([O-])(=O)=O FAKFSJNVVCGEEI-UHFFFAOYSA-J 0.000 description 1
- HPGGPRDJHPYFRM-UHFFFAOYSA-J tin(iv) chloride Chemical compound Cl[Sn](Cl)(Cl)Cl HPGGPRDJHPYFRM-UHFFFAOYSA-J 0.000 description 1
- XWKBMOUUGHARTI-UHFFFAOYSA-N tricalcium;diphosphite Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]P([O-])[O-].[O-]P([O-])[O-] XWKBMOUUGHARTI-UHFFFAOYSA-N 0.000 description 1
- PYOOBRULIYNHJR-UHFFFAOYSA-K trichloroholmium Chemical compound Cl[Ho](Cl)Cl PYOOBRULIYNHJR-UHFFFAOYSA-K 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000012856 weighed raw material Substances 0.000 description 1
- 239000002023 wood Substances 0.000 description 1
- 229910003454 ytterbium oxide Inorganic materials 0.000 description 1
- 229940075624 ytterbium oxide Drugs 0.000 description 1
- CKLHRQNQYIJFFX-UHFFFAOYSA-K ytterbium(III) chloride Chemical compound [Cl-].[Cl-].[Cl-].[Yb+3] CKLHRQNQYIJFFX-UHFFFAOYSA-K 0.000 description 1
- VNDYJBBGRKZCSX-UHFFFAOYSA-L zinc bromide Chemical compound Br[Zn]Br VNDYJBBGRKZCSX-UHFFFAOYSA-L 0.000 description 1
- NWONKYPBYAMBJT-UHFFFAOYSA-L zinc sulfate Chemical compound [Zn+2].[O-]S([O-])(=O)=O NWONKYPBYAMBJT-UHFFFAOYSA-L 0.000 description 1
- 229960001763 zinc sulfate Drugs 0.000 description 1
- 229910000368 zinc sulfate Inorganic materials 0.000 description 1
- ZVWKZXLXHLZXLS-UHFFFAOYSA-N zirconium nitride Chemical compound [Zr]#N ZVWKZXLXHLZXLS-UHFFFAOYSA-N 0.000 description 1
- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
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Abstract
Description
200904946 九、發明說明： 【發明所屬之技術領域】 本發明係關於發綠光螢光物質、其製造方法以及使用 該物質之發光裝置。 【先前技術】 發光二極體具有高發光效率且可發出鮮盤的色彩，所 以發光二極體可作為多樣之指示燈與發光源。 但因為發光二極體具有良好之單色峰波長，所以難以 作為白光發光二極體。 因此，已有揭露結合發紫外％二極體與發光物質以發 出白光之技術，此白光係由發紫外光二極體所發出的光以 及因受上述之發紫外光二《的激發而I螢光物質發光 —者混合而得。200904946 IX. Description of the Invention: [Technical Field] The present invention relates to a green-emitting phosphor, a method for producing the same, and a light-emitting device using the same. [Prior Art] The light-emitting diode has high luminous efficiency and can emit the color of a fresh disk, so that the light-emitting diode can be used as a variety of indicator lights and light sources. However, since the light-emitting diode has a good monochromatic peak wavelength, it is difficult to use it as a white light-emitting diode. Therefore, there has been disclosed a technique of combining a UV-emitting diode and a luminescent substance to emit white light, which is a light emitted by an ultraviolet light-emitting diode and an I-emitting substance excited by the ultraviolet light of the above-mentioned ultraviolet light. Luminescence - mixed.
此外，尚有利用二階激發而得到白光之技術，如利用 因紫外光二極體來激發發藍光物質以及藉此發藍光物質 所激發之藍光而激發YAG螢光物質來獲得白光。 然而，此二階激發方法難以得到高發光效率的白光。 因此，還有人發展出三波長型白光發光裝置，此裝置 係、纟σ合發紫外光二極體、發藍光物質、發綠光物質以及 發紅光物質，其中該發綠光物質為一氧化物螢光物質，如 以稀土元素做為發射中心。 但卻沙有發綠光氮氧化物螢光物質的研發，雖然已有 研究揭露發綠光氮氧化物螢光物質，如在日本專利號In addition, there are techniques for obtaining white light by second-order excitation, such as the use of an ultraviolet light source to excite a blue light-emitting substance and thereby a blue light excited by a blue light substance to excite a YAG fluorescent substance to obtain white light. However, this second-order excitation method is difficult to obtain white light with high luminous efficiency. Therefore, some people have developed a three-wavelength type white light emitting device, which is a 纟 合 紫外 ultraviolet light dipole, a blue light emitting material, a green light emitting material, and a red light emitting material, wherein the green light emitting material is an oxide. Fluorescent substances, such as rare earth elements as the emission center. However, there has been research and development of green nitrous oxide fluorescent substances in sand, although studies have revealed the emission of green nitrous oxide fluorescent substances, such as in the Japanese patent number.
2138-9748-PF 5 200904946 2005-2481 84之内容，但其發光效率還是未如其它之勞光 物質高。 本發明係與此問題相關，且提供一種具高發光效率之 發綠光氮氧化物螢光物質，也就是本發明的目的之一就是 提供一種發綠光螢光物質，其係藉由吸收發紫外光二極體 所發出的光而在螢光波長區發出高螢光效率的光。 此外，本發明尚提供一種發綠光螢光物質的製造方 法。 再者，本發明尚提供一種使用該發綠光螢光物質且具 高度發光效率的發光裝置。 【發明内容】 本發明之發綠光螢光物質係由一般式（1)表示： MlwReaM2x〇yNz (1) 其中Ml為第二族το素或sn之金屬元素，M2為第四族 元素除Sn之金屬元素，Re為活化元素，且a、x、y、z 與w為符合下列範圍之數字： 〇. 01 < a < 0. 20, 0-8 < χ/(w+a) < 1.0, 〇<z/y < 1. 0 。 且發綠光螢光物質也由一般式（1 )描述之：2138-9748-PF 5 200904946 2005-2481 84 content, but its luminous efficiency is still not as high as other luminous materials. The present invention relates to this problem, and provides a green light oxynitride fluorescent material having high luminous efficiency, that is, one of the objects of the present invention is to provide a green fluorescent material which is absorbed by absorption. The light emitted by the ultraviolet light source emits light of high fluorescence efficiency in the fluorescent wavelength region. Further, the present invention provides a method of producing a green-emitting phosphor. Furthermore, the present invention provides a light-emitting device using the green-emitting phosphor and having high luminous efficiency. SUMMARY OF THE INVENTION The green light-emitting phosphor of the present invention is represented by the general formula (1): MlwReaM2x〇yNz (1) wherein M1 is a metal element of a second group of τ or s, and M2 is a fourth group element other than Sn. The metal element, Re is an activating element, and a, x, y, z, and w are numbers in the following ranges: 〇. 01 < a < 0. 20, 0-8 < χ/(w+a) < 1.0, 〇 <z/y < 1. 0 . The green fluorescent substance is also described by the general formula (1):
MlwReaM2x〇yN2 (1) 其中Ml為第二族兀素或sn之金屬元素，M2為第四族 元素除Sn之金屬元素，Re為活化元素，且a、x、y、z 2138-9748-pp 200904946 與W為符合下列範圍之數字： 0. 01 < a < 0. 20, 0.8 < x/(w + a) < 1, 0<z/y < 1.0, 本發明之製造發綠光螢光物質的方法包括：將金屬MlwReaM2x〇yN2 (1) where Ml is a metal element of the second group of halogen or sn, M2 is a metal element of the fourth group element except for Sn, Re is an activating element, and a, x, y, z 2138-9748-pp 200904946 and W are numbers in accordance with the following ranges: 0. 01 < a < 0. 20, 0.8 < x / (w + a) < 1, 0 < z / y < 1.0, manufacturing of the present invention The method of green fluorescent material includes: metal
Ml、金屬M2與活化劑Re的金屬或上述金屬之金屬化合物 以符合-般式(1)的X肖w比例混合，以完成原料粉末之 製備；在一加壓條件下燒結該原剩_粉末，以得至]以一般式 (1)描述之發綠光螢光物質。 本發明之發光裝置係 '利用上述之發綠光營光物質與 發紫外光二極體，其中該發紫外光之二極體係為該蟹光物 質的激發光源。 本發明之申請係基於巴黎公約所主張之優先權 先權係於謂年6月25號向曰本專利局所提交之曰本專 利申請號2007-1 67007之宰，盆4』 杀其包括本案所描述之專利、Ml, metal M2 and the metal of the activator Re or the metal compound of the above metal are mixed in a ratio of X XI of the general formula (1) to complete the preparation of the raw material powder; sintering the raw _ powder under a pressurized condition , in order to obtain the green light fluorescent substance described by the general formula (1). The illuminating device of the present invention utilizes the above-mentioned green light camping light substance and ultraviolet light emitting diode, wherein the ultraviolet light generating diode system is an excitation light source of the crab light material. The application of the present invention is based on the priority of the Paris Convention, which is based on the patent application No. 2007-1 67007 submitted to the Patent Office on June 25th. The described patent,
說明書與圖示之内容。 本發明之發綠光榮光物質且 員具有尚度發光效率。且本發 明之發綠光螢光物質的製方法 x 從^ 乃/去可製造出具高發光效率的 發綠光螢光物質。 【實施方式】 [發綠光螢光物質] —般式（1)表示之 本發明之發綠光螢光物質係由 MlwReaM2x〇yNz (1) 2138-9748-PF 7 200904946The contents of the manual and the illustration. The green luminescent material of the present invention has a good luminous efficiency. Further, the method for producing a green-light fluorescent material of the present invention x can produce a green-emitting fluorescent material having high luminous efficiency from ^. [Embodiment] [Green-emitting fluorescent substance] - The general green light-emitting substance of the present invention is represented by MlwReaM2x〇yNz (1) 2138-9748-PF 7 200904946
0.01 < a < 0.20 知元素或Sn之金屬元素，M2為第四族 :素’ Re為活化元素，且a、 〇.8 < x/(w+a) < i 0<z/y < 1_ 〇。0.01 < a < 0.20 The metal element of the element or Sn, M2 is the fourth group: the prime 'Re is the active element, and a, 〇.8 < x/(w+a) < i 0<z/ y < 1_ 〇.
Ml 係擇自由 Ca、Ba、Sr、Mg、Ml is free to Ca, Ba, Sr, Mg,
Er 、 Tm 、 Yb 、 Lu 、 Μη 、 在式（1 )之較佳情況中， Zn與Sn所組成之族群之一 由Si、Ge、Zr與Ti所知a」 、INd、Sm、Eu、Gd、Tb、Dy、Ho、 B i與Sb所組成之族群之一或以上 之元素。 本發明之發綠光螢光物質具有波長不小於3〇〇 nm但 也不超過400 nm的激發帶。 發綠光螢光物質係由下列一般式（丨）表示之：Er, Tm, Yb, Lu, Μη, in the preferred case of the formula (1), one of the groups consisting of Zn and Sn is known by Si, Ge, Zr and Ti a", INd, Sm, Eu, Gd An element of one or more of the groups consisting of Tb, Dy, Ho, B i and Sb. The green-emitting phosphor of the present invention has an excitation band having a wavelength of not less than 3 Å nm but not more than 400 nm. The green-emitting fluorescent substance is represented by the following general formula (丨):
MlwReaM2x〇yNz (1) 其中Ml為第二族元素或Sn之金屬元素，M2為第四族 凡素除Sn之金屬元素，Re為活化元素，且a、x、y、z 與w為符合下列範圍之數字： 〇. 01 < a < 0. 20, 0.8 < x/(w + a) < 1, 0<z/y < 1.0, 本發明之製造發綠光螢光物質的方法包括：將金屬 Ml、金屬M2與活化劑Re的金屬或上述金屬之金屬化合物 2138-9748-PF 8 200904946 以符合-般式⑴的x肖 P ^ 匕例/fc匕合，以完成原料粉末之 I備’在_加壓條件士 rn,+,., ^ & m π亥原料粉末，以得到以一般式 (1)榣述之發綠光螢光物質。 今合步驟中之金屬M1為包括第二族元素… 金^素’且較佳擇自由Ca、Ba、Sr、Mg、Zr^如所 組成之族群之一或以t 之疋素’可使用上述金屬之金屬或 金屬化合物，若使用今M各 屬化合物’較佳使用其氧化物或氮 化物’最佳係使用其氮化物。 金屬Μ1的氮化物可益山士 — 物了精由在氬氣等惰性氣體下研磨金 屬Ml且在氮氣下氮化之而得，如當金屬[為約時，金屬MlwReaM2x〇yNz (1) where Ml is a metal element of the second group element or Sn, M2 is a metal element of the fourth group of all elements except for Sn, Re is an activating element, and a, x, y, z and w are in accordance with the following The number of the range: 〇. 01 < a < 0. 20, 0.8 < x / (w + a) < 1, 0<z/y < 1.0, the green light-emitting substance of the present invention The method comprises: combining the metal M1, the metal M2 with the metal of the activator Re or the metal compound 2138-9748-PF 8 200904946 of the above metal to meet the general formula (1) x P P ^ / / fc to complete the raw material powder I prepare a raw material powder of rn, +, ., ^ & m π in the _ pressurization condition to obtain a green light-emitting substance described in the general formula (1). The metal M1 in the present-combining step is a material including a second-group element... a metal compound, and preferably a free group of Ca, Ba, Sr, Mg, Zr^, or a halogen group of t. A metal metal or a metal compound, if a compound of the present M is used, it is preferred to use its oxide or nitride to use its nitride. The nitride of the metal ruthenium 1 can be obtained by grinding the metal M1 under an inert gas such as argon and nitriding under nitrogen, such as when the metal is about
Ml的氮化物可藉_置於，，吖、5 6小時而得， 其中金屬ΜΙ ό勺原料較佳為純的金屬，但其也可使用金屬 M1之吡唑（imide)化合物、氨化物（amide c⑽pound)、氧 化物寺作為其原料。 巫屬Μ1除為氧化物和氮化物外，還可以是碳酸鹽 (carbonates)、硫酸鹽（sulfates)、亞硫酸鹽 (sulfites) 氯化物（halides)、過氯酸鹽 (perchlorates)、過氧化物（per〇xides)等。更具體地， 這些化合物如包括碳酸I弓（calcium carb〇nate (CaC〇3))、 亞氯酸鈣（calcium chlorite (Ca(Cl〇2)2))、亞硫酸鈣 (calcium sulfite (CaS〇3))、亞攝酸妈（calcium phosphite (CaPH〇3)) 、 |g 石夕酸約(calcium aluminosilicate (CaO· AI2O3))、過氣酸 #5 (calcium perchlorate (Ca(Cl〇4)2))等含鈣化合物；碳化鋇（barium 2138-9748-PF 9 200904946 carbonate (BaC〇3))、硫酸鎖（barium sulfate (BaS〇4))、 氣化鎖（barium chloride (BaCl〗））、石肖酸鎖（barium nitrate (BaNCh))、氫氧化鋇（barium hydride (Ba (0H)2))、過氧化鋇（barium peroxide)等含鋇化合物；碳 化在(strontium carbonate (SrC〇3))、硫酸链（strontium sulfate (SrSCh))、溴化銷（strontium bromide (SrBn)) 等含錄化合物；破酸錢（magnesium carbonate (MgCOs))、 石;il 酉义鎮（magnesium sulfate (MgSCh))、演化鎮（magnesium bromide (MgBr2))等含鎂化合物；綠化鋅（zinc ch丨oride (ZnCh))、酸酸鋅（zin(： carbonate (ZnCCh))、硫酸辞（zinc sulfate (ZnSCK))、漠化鋅（zinc bromide (ZnBr2))等含 辞化合物；還有錫化物，如氣化錫（tin chloride (SnCl2)) 與硫酸錫（t i n su 1 f ate (SnSCU))。上述之化合物可單獨或 結合兩種或以上使用。 用於混合步驟中之金屬M2為包括第四族元素除Sn之 金屬元素’且較佳擇自由Si、Ge、Zr與Ti所組成之族群 之一或以上之元素，可使用上述金屬之金屬或金屬化合 物’雖然金屬M2的原料較佳為金屬簡單物質，但氧化物 和氮化物也可作為其金屬化合物原料。更具體地，可使用 氮化矽（Si3N4)、氧化矽（Si〇2)、一氧化鍺（germanium monoxide (GeO))、氧化鍺（germanium dioxide (GeCh))、 氧化鍅（zirconium oxide (Zr〇2))、氧化鈦（titanium oxide (Ti〇2))等' 氮化鍺（germanium nitride (GesNO)、 氮化錘（zirconium nitride (ZrN))、氮化鈦（titanium 2138-9748-PF 10 200904946 或結合兩種或以上 ’更明轉地，可使 nitride (TiN))等，這些化合物可單獨 使用車又佳與氧化物與氮化物合併使用 用氮化矽（SiD與氧化矽（Si〇 在氬氣等惰性 ’如當金屬M2 800~ 1 200〇C ' 如同金屬Ml，金屬M2的氮化物可藉由 氣體下研磨金屬M2且在氮氣下氮化之而得 為矽時，金屬M2的氮化物可藉由將矽置於 5〜6小時而得。 金屬M2的化合物也可為吼nMimide)化合物與氨化物 (awde c〇mpound) ’如將叫随2)2與M2的氧化物與氮化 物一起使用。 在混合步驟中所使用的活化劑較佳為擇自由[a、Ce、 Pr、Nd、Sm、Eu、Gd、Tb、Dy、H〇、Er、Tm、几、Lu、Mn、 B!與Sb所組成之族群之-或以上之元素，純金屬可作為 這些活化劑的原料，此外，也可使用函化物、吡唑（imide) 化合物、氨化物（amide corapound)、氧化物等作為活化劑 的原料，其中_化物可為氯化物或氟化物等，這些活化劑 可使用商業上可得之高純度原料’更明確地，這些活化劑 如包括乳化銪（EuCh)、氯化鋼（lanthanum chloride)、 硝酸鑭（lanthanum nitrate)、硝酸鈽（cerium nitrate)、 氯化鈽（cerium chloride)、硝酸鈽銨（ceric ammonium nitrate)、硝酸鈽二錢（ceric diammonium nitrate)、氧 化鐯（praseodymium oxide)、氣化镨（praseodymium chloride)、氯化敍（neodymium chloride)、氧化鈥 (neodymium oxide)、氯化釤（samarium chloride)、氯化 2138-9748-PF 11 200904946 此（gadolinium chloride)、氧化亂（gadolinium oxide)、 鼠化錢（terbium chloride)、氧化試（terbium oxide)、 氣化鋼（dysprosium chloride)、氧化鋼（dysprosium oxide)、氣化鈥（holmium chloride)、氧化鈥（holmium o x i d e)、氧化辑（e r b i u m o x i d e)、氯化録（t h u 1 i u m chloride)、氧化録（thulium oxide)、氧化鏡（ytterbium oxide)、氣化镱（ytterbium chloride)、氧化縳（lutetium oxide)、氣化猛（manganese chloride)、硝’酸猛（manganese nitrate)、硫酸錳（manganese sulfate)、碳酸錳 (manganese carbonate)、硫酸鉍（bismuth sulfate)、氧 化鉍（bismuth oxide)、氫氧化鉍（bismuth hydroxide)、 三氣化銻（antimony trichloride)、五氧化二銻（antim〇ny pentaoxide)、三氧化二錄（antimony trioxide)與硫酸錄 (antimony sulfate)。 在混合步驟中，所使用的原料較佳包含一助溶物質 (fluxing material)，以促進螢光物質在燒結步驟中之顆 粒的結晶成長。助熔物質的選擇可根據金屬M1、M2與活 化劑Re來決疋’如助炼物質可包括由化銨（amm〇nium halides) ’ 如氣化銨（NH4C1) ; i 化鋁（aiuminum hal ides)，如氟化鋁（aluminum fluoride (A1F3));鹼金 屬碳酸物，如碳酸鈉（NaC〇3)與碳酸鋰（Lic〇3);鹼金屬鹵 化物，如氣化鋰（LiCl)、氣化鈉（Naci)與氣化鉀（KC1); 驗土金屬鹵化物，如氣化鈣（CaCM、氟化鈣（CaF2)與and 說化鋇（BaFz);硼酸鹽化合物’如β2〇3、Η3β〇3與NaB4〇7 ; 2138-9748-PF 12 200904946 以及知酸鹽，如Li3P〇4與贿必p〇4。 在混合步驟中，弋 〇 01 < 式子（丨）令的a、x與w將符合： υ·ϋ1 - a ^ 0.20, 0. 8 < x/(w+a) < 〇5 金屬Ml、M2與活化劑以 瑙或礬土製成的研缽 ？、"與w的量在如以瑪 備原料粉末，此、、θ人 仃“里的研磨與混合’以製 此叱合步驟較佳以乾燥 不需移除溶劑了。杏 'χ進仃之，如此就 (acetone)、！丙田*劑時’可使用水、丙酮 (ethanol)等 ^ 〇Pr〇Pyi alC〇h〇1 ΠΡΑ))、乙醇 、但較佳使用有機溶劑，如丙酮。 :使用溶劑時’可採用加入氧化錯― 至有機溶劑以及秤量過的原料令，且將其置 球磨機(baU mi⑴進行混合 、：成的 ，、此《日f間較佳長於1小 1* ’但不要超過2 4小時0 a、日人 ，在此&步驟結束後，將氧化锆 師網/刀離出’且進行乾燥處理移除有機溶劑，即興得 原料粉末。當使用氣化飼作為上述金屬Ml之化合物：， 較佳於乾式混合步驟裡單獨使用氮化舞；在濕式混合步驟 中，較佳……化合物，如碳酸編lClum carbonate)與氯化鈣（calcium chl〇rite)。 當氮化石夕（Si.)與氧化石夕（训2)作為金屬M2時，較 佳在之前先以氮化矽與氧化矽在壓力為〇 9 Mpa的條件下 反應成0-N型態的前驅物，例如，混合金屬M1的氮化 物與具有Si—0-N型態前驅物的活化劑Re，以製備原料粉 末；當使用金屬M2氮化物時，氮化矽會在燒結步驟中分The nitride of Ml can be obtained by placing, 吖, and 5 6 hours, wherein the metal ruthenium spoon material is preferably a pure metal, but it can also use a metal M1 pyride compound, an amide ( Amide c (10) pound), oxide temple as its raw material. In addition to oxides and nitrides, the genus 巫1 can also be carbonates, sulfates, sulfites, halides, perchlorates, peroxides. (per〇xides) and so on. More specifically, these compounds include, for example, calcium carb〇nate (CaC〇3), calcium chlorite (Ca(Cl〇2)2), calcium sulfite (CaS〇). 3)), calcium phosphite (CaPH〇3), |g calcium aluminosilicate (CaO· AI2O3), calcium perchlorate (Ca(Cl〇4)2 )) and other calcium-containing compounds; barium carbide (barium 2138-9748-PF 9 200904946 carbonate (BaC〇3)), barium sulfate (BaS〇4), gasification lock (barium chloride (BaCl)), Barium nitrate (BaNCh), barium hydride (Ba (0H)2), barium peroxide, etc.; strontium carbonate (SrC〇3) , strontium sulfate (SrSCh), strontium bromide (SrBn) and other recorded compounds; magnesium carbonate (MgCOs), stone; il nes 镇 (magnesium sulfate (MgSCh)) Magnesium bromide (MgBr2) and other magnesium-containing compounds; zinc chororide (ZnCh), zinc (zin) Bonate (ZnCCh)), zinc sulfate (ZnSCK), zinc bromide (ZnBr2) and other compounds; and tin compounds such as tin chloride (SnCl2) and tin sulfate (tin su 1 f ate (SnSCU)). The above compounds may be used singly or in combination of two or more. The metal M2 used in the mixing step is a metal element including a group IV element other than Sn' and preferably free Si The element of one or more of the group consisting of Ge, Zr and Ti may be a metal or a metal compound of the above metal. Although the material of the metal M2 is preferably a simple metal substance, oxides and nitrides may also be used as the metal. More specifically, niobium nitride (Si3N4), niobium oxide (Si〇2), germanium monoxide (GeO), germanium dioxide (GeCh), zirconium oxide (Zr〇2)), titanium oxide (titanium oxide (Ti〇2)), etc. 'germanium nitride (GesNO), zirconium nitride (ZrN), titanium nitride (titanium 2138-9748- PF 10 200904946 or combine two or more 'more clearly It can be used for nitride (TiN), etc. These compounds can be used alone and in combination with oxides and nitrides using tantalum nitride (SiD and yttria (Si〇 is inert in argon, such as when metal M2 800~ 1 200〇C ' Like metal M1, the nitride of metal M2 can be obtained by grinding metal M2 under gas and nitriding under nitrogen, and the nitride of metal M2 can be placed by 5~6 hours. And got it. The compound of the metal M2 may also be a 吼nMimide compound and an amide (awde c〇mpound) such as an oxide and a nitride which are called 2) 2 and M2. The activator used in the mixing step is preferably free [a, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, H〇, Er, Tm, several, Lu, Mn, B! and Sb As the activator, a pure metal may be used as a raw material of these activators, or a functional compound, an imide compound, an amide corapound, an oxide or the like may be used as an activator. Raw materials, wherein the _ compounds may be chlorides or fluorides, etc., and these activators may use commercially available high-purity raw materials. More specifically, these activators include, for example, emulsified lanthanum (EuCh), lanthanum chloride. , lanthanum nitrate, cerium nitrate, cerium chloride, ceric ammonium nitrate, ceric diammonium nitrate, praseodymium oxide, gas Praseodymium chloride, neodymium chloride, neodymium oxide, samarium chloride, chlorinated 2138-9748-PF 11 200904946 (gadolinium chloride), oxidative disorder (gadolini Um oxide), terbium chloride, terbium oxide, dysprosium chloride, dysprosium oxide, holmium chloride, holmium oxide, oxidation Erbiumoxide, thu 1 ium chloride, thulium oxide, ytterbium oxide, ytterbium chloride, lutetium oxide, manganese chloride ), nitrate 'manganese nitrate, manganese sulfate, manganese carbonate, bismuth sulfate, bismuth oxide, bismuth hydroxide, triple gasification Antimony trichloride, antim〇ny pentaoxide, antimony trioxide and antimony sulfate. In the mixing step, the raw material used preferably contains a fluxing material to promote the crystal growth of the particles of the phosphor in the sintering step. The choice of fluxing material can be determined according to the metals M1, M2 and the activator Re. For example, the auxiliary material can include amm〇nium halides such as ammonium sulfate (NH4C1); i. aluminum (aiuminum hal ides) ), such as aluminum fluoride (A1F3); alkali metal carbonates, such as sodium carbonate (NaC〇3) and lithium carbonate (Lic〇3); alkali metal halides, such as lithium carbonate (LiCl), gas Sodium (Naci) and potassium hydride (KC1); soil metal halides such as calcium carbonate (CaCM, calcium fluoride (CaF2) and and bismuth (BaFz); borate compounds such as β2〇3, Η3β〇3 and NaB4〇7; 2138-9748-PF 12 200904946 and the acid salt, such as Li3P〇4 and bribe p〇4. In the mixing step, 弋〇01 < formula (丨) order a, x and w will be in accordance with: υ·ϋ1 - a ^ 0.20, 0. 8 < x/(w+a) < 〇5 Metal Ml, M2 and activator made of mortar or earthy mortar?, " And the amount of w is in the grinding and mixing of the raw material powder, such as θ 仃 以, in order to make the splicing step better to dry without removing the solvent. So (acetone), ! Water, acetone, etc., 〇Pr〇Pyi alC〇h〇1 ΠΡΑ)), ethanol, but preferably an organic solvent such as acetone is used. When a solvent is used, 'addition of oxidative error to organic solvent and Weighed raw materials, and put them in a ball mill (baU mi (1) mixed, :, this "day f is better than 1 small 1 * ' but not more than 2 4 hours 0 a, Japanese, here & After the end of the step, the zirconia mesh/knife is separated and dried to remove the organic solvent, and the raw material powder is obtained. When the gasification feed is used as the compound of the above metal M1, it is preferable to separate in the dry mixing step. Nitriding dance is used; in the wet mixing step, preferably ... compounds such as carbonic acid and calcium chloride (calcium chl carbonate). When nitrided silicon (Si.) and oxidized stone eve (train 2 When the metal M2 is used, it is preferred to react the tantalum nitride and the yttria with a pressure of 〇9 Mpa to form a 0-N type precursor, for example, a nitride of the mixed metal M1 and have Si— Activator Re of the 0-N type precursor to prepare raw material powder When a metal M2 nitride, silicon nitride in the sintering step will carve
2138-9748-PF 200904946 解’這對得到高紳许B a 、’ χ且具目表組成之發綠光螢光物質會有 :險：因此’較佳抑制s咖_驅物的分解，以獲 付較面純度的發綠光螢先物質。 在通後的-j：儿結步驟中，在混合步驟中所製備的原料粉 末會在加歷條件下進行燒結，所得之表示發綠光螢光物質 之一般式⑴裡的…”、…符合下列條件： 0. 01 < a < 0. 20, 〇. 8 < x/(w + a) <i.〇, 〇<z/y s 1· 〇 。 在製備原料粉来^的.、日人jW , 木的此合步驟中，金屬Ml、M2與活化 劑的比：符合式子⑴中的a、X與w的比例，且在燒結步 :中错由在含乳氣與氮氣的環境下燒結此原料粉末，而 得到符合式子（1)組成之發綠光螢光物質。 藉由將所得之原料粉末填入耐熱容器中，此耐熱容写 如為以氮化删(b〇ronnitride)、礬土 (alumina)或铺 成的掛伽ucible)與淺盤(tray)，再將其置於電爐等… 備中，料入氨氣以及還原氣體，如氣氣與氮氣之混合氣 體或-氧化碳氣體還原氣體，來進行原料粉末的燒結。 加熱時的壓力較佳大於U0大氣壓，且不要超過 1.50大氣壓’更佳w.02〜L3大氣壓，最佳為"5] 2 t氣麼。若此壓力不小力u0大氣壓，即可抑制反應速 率的下降此壓力不大於1.5G A氣壓，在電爐中賴 力條件就容易控制，也不需要固體設備。 此燒結溫度較佳為1 000。卜刚。C，更佳為1100t 2138-9748-PF 14 200904946 ' 1 350V的降低； 化。 。若燒結溫度不低於l〇〇(TC , 若燒結溫度不高於1 4 0 01：，就 就可抑制反應速率 可避免反應的無用 燒結時間較佳為3〜1 0小時。 並對燒結後的物 貝再進行一次或 在燒結結束後，較佳使之緩慢冷卻， 質進行研磨，且可對此研磨且燒結過的物 多次之燒結步驟。 所得之發綠光螢光物質較佳具有2G〜22“m之平均 顆拉尺寸’更佳為8。~16。㈣。若其平均顆粒尺寸不小於 ?，則所得之發綠光發光物質會具有較適當的強 度，若其平均顆粒尺寸不大 八也， 了不大於220 # m，則該螢光物質可 刀政地更均勻，所以當此螢 蛩九物貝與其它螢光物質混用 時，就可抑制不均勻的光產生。 (Cas. 9tEu〇. 〇3Si 8〇!〇N (Ca2.97EU0.03Si3〇4.5N3.( (Ca2.97Eu〇.〇3Si3〇6.〇N2.( (ca2.97EU0.03si2.7o3.9N: (Ca2.97Eu〇.03Si2.4〇3.1N； (ca2.97EU0.03si2.4o4.8N: 更明確地，本發明之發綠光榮光物質的例子包括： η ^ 1? 1 t Ο * A 1， 、 (Ca2.97Eu〇.〇3Si3〇3.6N3.6) 、 cca2.97EUO.03si305.4N2.4) 、 (ca2.97EU0.03si2.7o3.4N3.4)、 (ca2.97EU0.03si2.7o4.8N2.4)、 (ca2.97EUO.03si2.404.2N2.4)與 本發明之發綠 (Ca2.97Eu〇.〇3Ge3.〇〇3.6N3.6 (Ca2.97EU0.03Ti3.0O3.6N3. 6 (Ba2.97Euo.03Ge3.oO3.eN3.0 光榮光物質的例子尚包括 ， CCa2.97Eu〇.〇3Zr3.0〇3.6N3.6) (Ba2.97Euo.03Si3.oO3.6N3. 6) (Ba2.97Eu〇.03Zr3.0〇3.6N3.6)2138-9748-PF 200904946 The solution is that the green-emitting fluorescent material that is composed of 绅 绅 a a ' 具 具 具 具 具 具 具 具 具 具 具 具 : : : : : : : : : : : : : : : : 较佳 较佳 较佳 较佳 较佳A greenish light-emitting substance with a relatively pure purity is obtained. In the -j: knot step after the pass, the raw material powder prepared in the mixing step is sintered under the calendaring condition, and the obtained product represents the "..." in the general formula (1) of the green-emitting phosphor. The following conditions: 0. 01 < a < 0. 20, 〇. 8 < x/(w + a) <i.〇, 〇<z/ys 1· 〇. In the preparation of raw material powder , Japanese jW, wood in this combination, the ratio of metal Ml, M2 and activator: in accordance with the ratio of a, X and w in formula (1), and in the sintering step: in the wrong with The raw material powder is sintered in a nitrogen atmosphere to obtain a green-emitting phosphor material conforming to the composition of the formula (1). By filling the obtained raw material powder into a heat-resistant container, the heat-resistant capacity is written by nitriding ( B〇ronnitride), alumina or paved gamucible, and tray, and placed in an electric furnace, etc. In preparation, ammonia and reducing gases such as gas and nitrogen are mixed. The gas or the carbon oxide gas reduces the gas to sinter the raw material powder. The pressure during heating is preferably greater than U0 atmospheric pressure, and does not exceed 1.50 atmospheres' better w.02 L3 atmospheric pressure, the best is "5] 2 t gas. If this pressure is not small force u0 atmospheric pressure, it can suppress the decrease of reaction rate. This pressure is not more than 1.5GA pressure, and the pressure condition is easy to control in the electric furnace. No need for solid equipment. The sintering temperature is preferably 1 000. Bu Gang C, more preferably 1100t 2138-9748-PF 14 200904946 '1 350V reduction; If the sintering temperature is not lower than l〇〇 (TC If the sintering temperature is not higher than 1 4 01:, the reaction rate can be suppressed to avoid the useless sintering time of the reaction is preferably 3 to 10 hours. The sintered shell is again or after the sintering is completed. Preferably, the material is slowly cooled, the material is ground, and the ground and sintered material can be sintered several times. The resulting green light-emitting material preferably has an average particle size of 2G to 22"m". More preferably, it is 8.~16. (4) If the average particle size is not less than ?, the obtained green light emitting material will have a relatively suitable strength, and if the average particle size is not large, it is not more than 220 # m. , the fluorescent material can be more evenly knifed, so when When mixed with other fluorescent materials, it can suppress uneven light generation (Cas. 9tEu〇. 〇3Si 8〇!〇N (Ca2.97EU0.03Si3〇4.5N3.(Ca2.97Eu〇 .〇3Si3〇6.〇N2.( (ca2.97EU0.03si2.7o3.9N: (Ca2.97Eu〇.03Si2.4〇3.1N; (ca2.97EU0.03si2.4o4.8N: more specifically, this Examples of the green light-emitting substance of the invention include: η ^ 1? 1 t Ο * A 1, , (Ca2.97Eu〇.〇3Si3〇3.6N3.6), cca2.97EUO.03si305.4N2.4) , ( ca2.97EU0.03si2.7o3.4N3.4), (ca2.97EU0.03si2.7o4.8N2.4), (ca2.97EUO.03si2.404.2N2.4) and the green of the invention (Ca2.97Eu〇 〇3Ge3.〇〇3.6N3.6 (Ca2.97EU0.03Ti3.0O3.6N3. 6 (Ba2.97Euo.03Ge3.oO3.eN3.0 Examples of glorious light substances are also included, CCa2.97Eu〇.〇3Zr3. 0〇3.6N3.6) (Ba2.97Euo.03Si3.oO3.6N3. 6) (Ba2.97Eu〇.03Zr3.0〇3.6N3.6)
2138-9748-PF 15 200904946 (Ba2. 97EUO. 03T i 3. 0〇3. δΝ3. 6) 、 (Sr2. 97E110. 0 3 S i 3 .0〇3. (Sr2. 9 ϊΕ U 0 . 03〇63. 0〇3. 6N3. 6 ) (Sr2. 97E110. 03Zr 3 .0〇3. (Sr2. 97EUO. 03T i 3. 0〇3. 6N3. 6) 、 (Mg2. 97EU0. 0 3 S i 3 .0〇3. (Mg2. 97EUO. 03G63. 0〇3. 6N3. 0 、 (Mgz. qtEuo. 03ΖΓ3 .0〇3. (Mg2. 97EU0. 03T i 3. 0〇3. eN3. 6) 、 (ΖΠ2. 9 7 E u 〇 0 3S i 3 .0〇3. (Zm. 97EU〇. 03G63. 0〇3. eN3. 6 ) Λ (Ζΐΐ2. 97E110. 03ΖΓ3 .0〇3. (ΖΠ2. 97E110.03T i 3. 0〇3. eN3. δ) 、 (Sm. 97EU0. 03S i 3 .0〇3. (Sn2. 97EU0. 0 3 G e 3. 0〇3. 6N3. 0 > (Sri2.97E110.03ΖΓ3. c l〇3. 6 (Sn2. 97EU0. 〇3T i 3. 0〇3. 6N3. 6 )。 類似 地， 本發明之發綠光螢光物質的 例 (Caz. 97Eli〇. 0 3G 6 2 . 4〇4. δΝ 2. 〇) 、 (Ca2. 97EU0. 0 3 Z Γ 2 . .4〇4. (Ca2. 97EUO. 03T i 2. 4〇4. δΝ2. 〇) > (B&2. 97E110. 03S i 2. .4〇4. (BS2. 97EUO. 03G62. 4〇4. δΝ2. 〇) 、 (Ba2.97EU0.03. ΖΓ2. (Ba2. 97EUO. 03T i 2. 4〇4 . δΝ2. 〇) (Sr2. 97EU0. 03S i 2. 4〇4. (Sr2. 97EUO. 03G62. 4〇4. δΝ2. ◦), (Srz. 9 7EU0. 0 3 Z Γ2 . 4 〇4 . 8 (Sr2. 97EUO. 03T i 2. 4〇4. δΝ2. 〇) 、 (Mg2. 97EU0. 03' S12. (Mg2. 97EUO. 03G62. 4〇4 . δΝ2. ◦) Λ (Mg2. 97EU0. 03ΖΓ2. 4〇4. (Mg2. 97E110.03T i 2. 4〇4. δΝ2 . ◦) Ν (Zm. 97E110. 03S i 2. 4〇4 . (Zri2. 97E110. 03G62. 4〇4. δΝ 2 . 〇) 、 (Zm. 97E110. 03ΖΓ 2. 4〇4 · (Zn2. 97EU0. 03T i 2. 4〇4. δΝ 2 . ◦) 、 (Sm. 97E110. 03S i 2. 4〇4. (Sm. 97E110. 03G62, 4〇4. δΝ2. ◦)， (S112.97E110. 〇 3ΖΓ2. 4 〇4 . 8 (Sm. 97E110. 03T i 2. 4〇4. δΝ2. 0 )。 iN： 與 與 且本發明之發綠光螢光物質的例子包括 (Ca2.99EU0.0lGe3.0〇3.6N3. 6) 、 （Ca2.95EU〇.05Ge3.0〇3,6N3. 6) 2138-9748-PF 16 200904946 (C&2. 93EUO. 07G63. 0〇3. 6N3. θ) 、 （Ca2.9[)Eu〇.l〇Ge3.0〇3.6N3. 6) (Ca 2. 87EU〇. 13G63. 0〇3, 6N3. 6) 、 （Ca2.85EU0.15Ge3.0〇3.6N3. 6) (Ca2,83EU0.uGe3.0〇3.6N3.6)與（Ca2.8〇Ell〇.2〇Ge3.0〇3.6N3.6)。 本 I务明利用 La、Ce、Pr、Nd、Sm、Eu、Gd、Tb、Dy、 Ho、Er、Tm、Yb、Lu、Mn、Bi與Sb作為活化元素所製成 / 的發綠光螢光物質包 (Ca2. 97Ce〇. 03Si 3. 0〇3. 6N3. 6) (Ca2.97Nd0.03Si3.0O3.6N3. 6) (Ca2. 97Gd〇. 03S1 3. 0〇3. 6N3. β) (Ca 2.97 Dyo.osSis.oOs.eNs.e) (Ca2.97Er〇.〇3Si：3.0〇3.6N3. 6) (Ca2. 97Yb〇. 03S1 3. 0〇3. 6N3. θ) (Ca2. 97Mn〇. 03S i 3. 0〇3. 6N3. 6 ) (Ca2. 97Sb〇. 03S1 3. 0〇3. 6N3. θ) 括：(Ca2. 97La〇. 03S1 3. 0〇3. 6N3. 6) (Caz. 97ΡΓ0. 03S i 3. 0〇3. 6N3. 〇) (Ca2. 97SlIl〇. 03S i 3. 0〇3. 6N3. 6) 、 (Ca2. 97Tb〇. 03S i 3. 0〇3. 6N3. 0 、 (Ca2. 97H〇0. 03S i 3. 0 0 3 6N3. 6 ) Λ (Ca2. 97Tm〇· 03S i 3. 0〇3. 6N3. 6 ) 、 (Ca2. 97LU0.03S i 3. 0〇3. 6N3. e) (Ca2. 97B i 〇. 03S i 3. 0〇3. 6N3. 6 ) 與 且金屬元素Ml and M2可包括複數種金屬，如 (Bai. 〇Cai. 97E110.03S i 3. 〇〇3.6N3. β) 、 (Sri. 〇Cai. 97E110.03S13.0O3.6N3.6) (Sni. oCai. 97 Eu〇. 03S i 3. 〇〇3.6N3. e) 、 (Ca2.97E110.03S i 2. oGei. 0O3. θΝ3. θ)、 (Ca2.97ElI0.03Si2.0Zri.0O3.6N3. δ) Λ (Ca2. 97EU0. 03Sl2. 〇T ΐ 1. 0〇3. βΝ3. δ) Λ (Bai. 〇Sri. 〇Ca〇. 97EII0. 03S i 3. 0〇3. 6N3. 6)、（Sri, 〇Mgl. oCaQ, 97E1IQ. Q3S i 3. Q〇3. 6N3. 6)、 (Bai. 〇Sri. 〇Ca〇. 97E110.03S13. 〇Gei. 0O3.6N3. e) 與 (Sri. 〇Mgl. oGat). 97E1IG. G3Si3.GZri.D〇3.6?^3.6)。 [發光裝置] 本發明之發光裝置包括上述發綠光螢光物質與發紫 外光二極體，其中該紫外光二極體係為發綠光螢光物質的 2138-9748-PF 17 200904946 激發光源。 第9圖為本發明之一發光裝置的示意圖。在第9圖所 不之發光裝置111中’具有位於前端之透明基材101、 發光二極體1〇5、形成半圓狀且位於透明基材1〇1上之透 明樹脂體1 0 3。 會X發光二極體之紫外線而稍微惡化之透明樹脂體 1 03車乂佳以環氧樹脂（ep〇xy res丨ns)、氨基曱酸脂樹脂 (urethane resins)、石夕樹脂（siiicon resins)、聚苯乙 烤树月曰（polystyrene resins)、聚乙烯樹脂（polyvinyl ins) 乙稀型樹脂（polyethylene-based resins)、 l 丙稀型树脂（p〇ly pr〇pylene —based resins)等形成， 在這些樹脂中，較佳使用矽樹脂與環氧樹脂，因為它們可 使營光物質粉末均勻地分散。透明樹脂體的表面可被加工 成4兄面，使其表面具有鏡面功能；或可加工成透鏡，使表 面可使從發光裝置的光徑聚合或散射。 透明樹脂體10 3中含有螢光物質粉末1 〇 2，此螢光物 貝籾末1 02可由上述之發綠光螢光物質形成，更較佳包括 毛紅光螢光物質與發藍光螢光物質，以確保其顏色表現特 性（color rendering pr〇perties),此發紅光螢光物質與 發藍光螢光物質被發紫外光二極體1〇5激發而分別發出紅 螢光與藍螢光，混合由發光裝置所發出的光與由發綠光螢 光物貝所發出的綠光，以在顏色表現特性裡形成良好的白 光。發紅光螢光物質如包括..se : Eu、CaS : Eu、eaA1SiN3 : 心與La^s : Eu;發藍光螢光物質如包括：h (p〇4)3ci : 18 2138-9748-pp 2009049462138-9748-PF 15 200904946 (Ba2. 97EUO. 03T i 3. 0〇3. δΝ3. 6) , (Sr2. 97E110. 0 3 S i 3 .0〇3. (Sr2. 9 ϊΕ U 0 . 03〇 63. 0〇3. 6N3. 6 ) (Sr2. 97E110. 03Zr 3 .0〇3. (Sr2. 97EUO. 03T i 3. 0〇3. 6N3. 6) , (Mg2. 97EU0. 0 3 S i 3 .0〇3. (Mg2. 97EUO. 03G63. 0〇3. 6N3. 0 , (Mgz. qtEuo. 03ΖΓ3 .0〇3. (Mg2. 97EU0. 03T i 3. 0〇3. eN3. 6) , ( ΖΠ 2. 9 7 E u 〇0 3S i 3 .0〇3. (Zm. 97EU〇. 03G63. 0〇3. eN3. 6 ) Λ (Ζΐΐ2. 97E110. 03ΖΓ3 .0〇3. (ΖΠ2. 97E110.03T i 3. 0〇3. eN3. δ) , (Sm. 97EU0. 03S i 3 .0〇3. (Sn2. 97EU0. 0 3 G e 3. 0〇3. 6N3. 0 > (Sri2.97E110. 03ΖΓ3. cl〇3. 6 (Sn2. 97EU0. 〇3T i 3. 0〇3. 6N3. 6 ). Similarly, an example of the green-emitting phosphor of the present invention (Caz. 97Eli〇. 0 3G 6 2 4〇4. δΝ 2. 〇) , (Ca2. 97EU0. 0 3 Z Γ 2 . .4〇4. (Ca2. 97EUO. 03T i 2. 4〇4. δΝ2. 〇) >(B&2 97E110. 03S i 2. .4〇4. (BS2. 97EUO. 03G62. 4〇4. δΝ2. 〇) , (Ba2.97EU0.03. ΖΓ2. (Ba2. 97EUO. 03T i 2. 4〇4 . δΝ2. 〇) (Sr2. 97EU0. 03S i 2. 4〇4. (Sr2. 97EUO. 03G62. 4〇4. δΝ2. ◦), (Srz. 9 7EU0. 0 3 Z Γ2 . 4 〇4 . 8 (Sr2. 97EUO. 03T i 2. 4〇4. δΝ2. 〇) , (Mg2. 97EU0. 03' S12. (Mg2. 97EUO. 03G62. 4〇4 . δΝ2. ◦) Λ (Mg2. 97EU0. 03ΖΓ2. 4〇4 (Mg2. 97E110.03T i 2. 4〇4. δΝ2 . ◦) Ν (Zm. 97E110. 03S i 2. 4〇4 . (Zri2. 97E110. 03G62. 4〇4. δΝ 2 . 〇) , ( Zm. 97E110. 03ΖΓ 2. 4〇4 · (Zn2. 97EU0. 03T i 2. 4〇4. δΝ 2 . ◦) , (Sm. 97E110. 03S i 2. 4〇4. (Sm. 97E110. 03G62, 4〇4. δΝ2. ◦), (S112.97E110. 〇3ΖΓ2. 4 〇4. 8 (Sm. 97E110. 03T i 2. 4〇4. δΝ2. 0 ). iN: Examples of the green-emitting phosphor of the present invention include (Ca2.99EU0.0lGe3.0〇3.6N3.6), (Ca2.95EU〇.05Ge3.0〇3,6N3. 6) 2138- 9748-PF 16 200904946 (C& 2.93EUO. 07G63. 0〇3. 6N3. θ) , (Ca2.9[)Eu〇.l〇Ge3.0〇3.6N3. 6) (Ca 2. 87EU〇. 13G63. 0〇3, 6N3. 6) , (Ca2.85EU0.15Ge3.0〇3.6N3. 6) (Ca2,83EU0.uGe3.0〇3.6N3.6) and (Ca2.8〇Ell〇.2〇 Ge3.0〇3.6N3.6). This is a green glow that is made of La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Mn, Bi, and Sb as activating elements. Light substance package (Ca2. 97Ce〇. 03Si 3. 0〇3. 6N3. 6) (Ca2.97Nd0.03Si3.0O3.6N3. 6) (Ca2. 97Gd〇. 03S1 3. 0〇3. 6N3. β) (Ca 2.97 Dyo.osSis.oOs.eNs.e) (Ca2.97Er〇.〇3Si: 3.0〇3.6N3. 6) (Ca2. 97Yb〇. 03S1 3. 0〇3. 6N3. θ) (Ca2. 97Mn S. 03S i 3. 0〇3. 6N3. 6 ) (Ca2. 97Sb〇. 03S1 3. 0〇3. 6N3. θ) Included: (Ca2. 97La〇. 03S1 3. 0〇3. 6N3. 6) (Caz. 97ΡΓ0. 03S i 3. 0〇3. 6N3. 〇) (Ca2. 97SlIl〇. 03S i 3. 0〇3. 6N3. 6) , (Ca2. 97Tb〇. 03S i 3. 0〇3. 6N, 0, (Ca2. 97H〇0. 03S i 3. 0 0 3 6N3. 6 ) Λ (Ca2. 97Tm〇· 03S i 3. 0〇3. 6N3. 6 ) , (Ca2. 97LU0.03S i 3 0〇3. 6N3. e) (Ca2. 97B i 〇. 03S i 3. 0〇3. 6N3. 6 ) and the metal elements Ml and M2 may comprise a plurality of metals, such as (Bai. 〇Cai. 97E110. 03S i 3. 〇〇3.6N3. β) , (Sri. 〇Cai. 97E110.03S13.0O3.6N3.6) (Sni. oCai. 97 Eu〇. 03S i 3. 〇〇3.6N3. e) , ( Ca2 .97E110.03S i 2. oGei. 0O3. θΝ3. θ), (Ca2.97ElI0.03Si2.0Zri.0O3.6N3. δ) Λ (Ca2. 97EU0. 03Sl2. 〇T ΐ 1. 0〇3. βΝ3. δ) Λ (Bai. 〇Sri. 〇Ca〇. 97EII0. 03S i 3. 0〇3. 6N3. 6), (Sri, 〇Mgl. oCaQ, 97E1IQ. Q3S i 3. Q〇3. 6N3. 6) (Bai. 〇Sri. 〇Ca〇. 97E110.03S13. 〇Gei. 0O3.6N3. e) and (Sri. 〇Mgl. oGat). 97E1IG. G3Si3.GZri.D〇3.6?^3.6). [Light-emitting device] The light-emitting device of the present invention comprises the above-mentioned green-emitting phosphor and the ultraviolet light-emitting diode, wherein the ultraviolet light-emitting diode is a 2138-9748-PF 17 200904946 excitation light source that emits green fluorescent material. Figure 9 is a schematic view of a light-emitting device of the present invention. In the light-emitting device 111 of Fig. 9, the transparent substrate 101 and the light-emitting diode 1〇5 located at the front end are formed, and the transparent resin body 1 0 3 which is formed in a semicircular shape and located on the transparent substrate 1〇1 is formed. A transparent resin body which is slightly deteriorated by the ultraviolet ray of the X-ray diode. 203 乂 〇 环氧树脂 epoxy resin (ep〇xy res丨ns), urethane resins, siiicon resins , polystyrene resins, polyvinyl ins, polyethylene-based resins, and p〇ly pr〇pylene-based resins, Among these resins, enamel resins and epoxy resins are preferably used because they allow the camping substance powder to be uniformly dispersed. The surface of the transparent resin body can be processed into a four-sided surface to have a mirror surface function, or can be processed into a lens such that the surface can be polymerized or scattered from the light path of the light-emitting device. The transparent resin body 10 3 contains a fluorescent substance powder 1 〇 2, and the fluorescent material 籾 籾 1 102 can be formed by the above-mentioned green light-emitting substance, and more preferably includes a red-light fluorescent substance and a blue-emitting fluorescent substance. In order to ensure its color rendering characteristics (color rendering pr〇perties), the red-emitting phosphor and the blue-emitting phosphor are excited by the ultraviolet diode 1〇5 to emit red and blue fluorescent light respectively, mixed by The light emitted by the illuminating device and the green light emitted by the green luminescent phosphor form a good white light in the color expression characteristics. The red-emitting fluorescent substance includes: .se : Eu, CaS : Eu, eaA1SiN3 : heart and La^s : Eu; blue light-emitting substance such as: h (p〇4) 3ci : 18 2138-9748-pp 200904946
Eu、（Ba，Sr)MgAli〇〇i7 : Eu、Μη (Ba，Sr，Ca，Mg)i。（p〇4)5 Ch : Eu 與 ZnS : Ag。 除上述之發綠光螢光物質外，還可使用會被發紫外光 二極體激發而發出綠螢光的發綠光螢光物質，這些發綠光 螢光物質如包括：由銪激發鋁酸鹽的螢光物質，如 BaMg2Ali6〇27 : Eu'MnBaMgAhoOn : Eu, Μη;以及由銪激 發驗土金屬石夕酸氮化物（alkaline earth metal silicon oxynitride)的螢光物質，如（MgCaSrBa) Si2〇2N2 : Eu; 以及由銪激發驗土金屬石夕酸物（alkal ine earth metal silicate)的螢光物質’如 Ba2Si〇4:Eu。 這些螢光物質102較佳以〇.卜20 wt%分散於透明樹脂 體103中，更佳為〇·3~15 wt%。若螢光物質的含量小於 0 · 1 wt% ’就有可能會因透明樹脂體的吸收與散射而抑制 發光效率，若螢光物質的含量大於%就有可能因螢光 物質粉末的聚集而抑制發光效率。Eu, (Ba, Sr)MgAli〇〇i7 : Eu, Μη (Ba, Sr, Ca, Mg)i. (p〇4) 5 Ch : Eu and ZnS : Ag. In addition to the above-mentioned green light-emitting material, a green-emitting phosphor that emits green fluorescent light by being excited by an ultraviolet light-emitting diode may be used, and the green-emitting fluorescent materials include: a fluorescent substance of a salt such as BaMg2Ali6〇27: Eu'MnBaMgAhoOn: Eu, Μη; and a fluorescent substance such as (MgCaSrBa) Si2〇2N2 which is excited by an earth earth metal silicon oxynitride. : Eu; and a fluorescent substance such as Ba2Si〇4:Eu which activates the alkal ine earth metal silicate. These phosphors 102 are preferably dispersed in the transparent resin body 103 in an amount of 20 wt%, more preferably 3 to 15 wt%. If the content of the fluorescent substance is less than 0 · 1 wt% ', it is possible to suppress the luminous efficiency due to absorption and scattering of the transparent resin body, and if the content of the fluorescent substance is more than %, it may be suppressed by the aggregation of the fluorescent substance powder. Luminous efficiency.
InGaN、GaN、InAlGaN、AlGaN、BAlGaN、BinAlGaN 等可作為激發上述之螢光物質的發紫外光二極體。 透明樹脂體103中尚可包含一補充劑（extender)來 防止色彩的不均勻，而擴散劑（d丨f f us丨〇n叫印土）可增加 發紫外光二極體1 05所發出的定向紫外線而變小的視角， 鈦酸鋇（barium titanium)、氧化鈦（tltanium 〇xide)、 氧化铭Uluminuni oxide)、氧化矽等可作為擴散劑 (diffusion agent) 0 2138-9748-PF 19 200904946 例1 : ⑶。：丨广g的氮化釣(Ca3N2)、"51。g的氧化發 (EuC1)進^的氮化石夕（Sl3N〇與Q.Q192g的氯化銪 :進仃研磨與混合處理’以製備原料粉末；再將心 …、“分末填入氮化硼所製成的坩堝中于 的電爐中，，、，η , 丄罝7、死滿氣氣 以 ·大氣塵、匕350。0的條件燒結3小時， C ^ 勞光物質，此螢光物質的組成為InGaN, GaN, InAlGaN, AlGaN, BAlGaN, BinAlGaN or the like can be used as the ultraviolet light emitting diode for exciting the above-mentioned fluorescent substance. The transparent resin body 103 may further include an extender to prevent color unevenness, and the diffusing agent (d丨ff us丨〇n called printed soil) may increase the directional ultraviolet light emitted by the ultraviolet light emitting diode 05. For smaller viewing angles, barium titanium, titanium oxide (ttanium 〇xide), oxidized cerium oxide, cerium oxide, etc. can be used as a diffusion agent. 0 2138-9748-PF 19 200904946 Example 1: (3). : 丨广g's nitride fishing (Ca3N2), "51. The oxidized hair of g (EuC1) enters the nitrite of Xi (Sl3N〇 and Q.Q192g of lanthanum chloride: 仃 grinding and mixing treatment) to prepare the raw material powder; then the heart... In the electric furnace in which the crucible is made, η, 丄罝7, 死 气 以 大气 大气 大气 大气 大气 大气 大气 大气 大气 大气 大气 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 匕 , , , , , , , , , , Composition
Cas.97Euu3Si8〇uNl()。 為 ^量測所得之發綠光螢光物質的激發光譜與發射光 ::的發綠光榮光物質具有在波長為3〇°，“"付 ’其發射峰約為36G nm;對於發紫外光二極體 °所侍之發綠光螢光物質有效率地發光，且其發射光 二的發射峰具有…的半寬度(一一= 見的發射峰。此發綠光螢光物質之激發光譜顯示於第i 圖，而其發射光譜為第2圖。 例2 ·· 利用與例1相同的方式得到此例之榮光物質，但所使 的原枓有所不同：L 3711 §的氮化飼、1.0311 g的氧 二夕、〇.5350 §的氮化石夕、。.0739 g的氯化销與〇.〇3 g 总鼠化銨。再量測此螢光物質的激發光譜與發射光譜，此 螢光物質的組成為CU— 斤仔之發綠光螢光物質具有在波長為34〇〇腿附 的激發帶’其發射峰約為35〇nm;對於發紫外光二極體Cas.97Euu3Si8〇uNl(). The excitation spectrum and the emitted light of the green-emitting fluorescent material obtained by the measurement are: at a wavelength of 3 〇, """ the emission peak is about 36 G nm; The green light-emitting substance of the light diode is efficiently emitted, and the emission peak of the emitted light has a half width of (one to one = the emission peak seen. The excitation spectrum of the green-emitting fluorescent substance is displayed) In the figure i, the emission spectrum is shown in Fig. 2. Example 2 ·· The glory material of this example was obtained in the same manner as in Example 1, but the original enthalpy was different: the nitrogen feed of L 3711 § 1.0311 g of oxygen dioxide, 〇5350 § of the nitrite, .0739 g of chlorinated pin and 〇.〇3 g of total mutated ammonium. The excitation and emission spectra of this fluorescent substance are measured. The composition of the fluorescent substance is CU- jin 仔 之 绿 绿 具有 具有 具有 具有 具有 具有 具有 具有 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿 绿
2138-9748-PF 20 200904946 而《，所仔之發綠光螢光物質有效率地發籃綠光，且其發 射光譜的發射峰具有約97㈣的半寬度，故其具有寬的發 射峰。此發綠光勞光物質之激發光譜顯示於第3圖，而其 發射光譜為第4圖。 例3: 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同：U531 g的氮化約、g的氧 化石夕、0.3300 g的氮化石夕、〇 〇729 g的氯化銪與〇 忌 的氯化銨。再量測此螢光物質的激發光譜與發射光譜，此 勞光物質的組成為Ca2.97Eu〇.«3Si3〇4.5N3.。。 所仔之發綠光螢光物質具有在波長為300〜400 nm附 近的激發帶，其發射峰約為34〇_;對於發紫外光二極體 而5 ’所得之發綠光螢光物質有效率地發黃綠光，且其發 射光譜的發射峰具有約1〇7 nm的半寬度，故其具有寬的 毛射峰。此發綠光螢光物質之激發光譜顯示於第3圖，而 其發射光譜為第4圖。 例4 : 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同：1.3326 g的氮化鈣、1.5033 g的氧 化矽、0_13〇〇 g的氮化矽、0.0718 g的氯化銪與〇.〇3 g 的氯化知Γ °再量測此螢光物質的激發光譜與發射光譜，此 榮光物質的組成為Ca2.97Eu〇.D3Si3〇5.4N2.4。 2138-974 8-PF 21 200904946 所得之發綠光螢光物質具有在波長為3〇〇〜4〇〇 nm附 近的激發帶，其發射峰約為340 nm ;對於發紫外光二極體 而吕，所得之發綠光螢光物質有效率地發光，且其發射光 譜的發射峰具有約103 nm的半寬度，故其具有寬的發射 峰。此發綠光螢光物質之激發光譜顯示於第3圖，而其發 射光譜為第4圖。 例5 : 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同：丨· 3164 g的氮化鈣、1. 6500 g的氧 1匕矽、〇· 0709 g的氣化銪與〇· 03 g的氣化銨。再量測此 螢光物質的激發光譜與發射光譜，此螢光物質的組成為 CauduuaShOuL.。。 、所侍之發綠光螢光物質具有在波長為30 0〜4〇〇 nm附 、的激《▼，其發射峰約為330 nm ;對於發紫外光二極體 、、， 彳寸之發綠光榮光物質有效率地發光，且其發射光 4的發射峰具有約103 nm的半寬度，故其具有寬的發射 峰。此發綠光螢光物質之激發光譜顯示於第3圖，而其發 射光譜為第4圖。 ” x 例6 : 利用與例1相同的方式得到此例之螢光物質，但所使 Π原Γ有所不同：1.4472 g的氮化約、"15“的氧 8〇〇 g的氮化矽、0.0780 g的氣化銪與0.03 g2138-9748-PF 20 200904946 And, the green light-emitting substance emits green light efficiently, and the emission peak of the emission spectrum has a half width of about 97 (four), so that it has a broad emission peak. The excitation spectrum of this green light-emitting substance is shown in Fig. 3, and its emission spectrum is shown in Fig. 4. Example 3: The fluorescent material of this example was obtained in the same manner as in Example 1, except that the raw materials used were different: nitriding of U531 g, oxidized stone of g, 0.3300 g of nitriding cerium, 〇〇729 g of lanthanum chloride and jealous ammonium chloride. The excitation spectrum and the emission spectrum of the fluorescent substance are measured, and the composition of the working substance is Ca2.97Eu〇. «3Si3〇4.5N3. . The green-emitting fluorescent material has an excitation band around a wavelength of 300-400 nm, and its emission peak is about 34 〇 _; the green-emitting fluorescent material obtained by 5' for the ultraviolet light-emitting diode is efficient. The ground emits yellow-green light, and its emission spectrum has an emission peak with a half width of about 1 〇 7 nm, so it has a broad peak of the peak. The excitation spectrum of this green-emitting phosphor is shown in Fig. 3, and its emission spectrum is shown in Fig. 4. Example 4: The fluorescent material of this example was obtained in the same manner as in Example 1, except that the raw materials used were different: 1.3326 g of calcium nitride, 1.5033 g of cerium oxide, 0_13 〇〇g of cerium nitride, 0.0718 The osmium chloride of g and the chlorination of 〇.〇3 g Γ ° The excitation and emission spectra of this fluorescent substance were measured. The composition of this luminescent material was Ca2.97Eu〇.D3Si3〇5.4N2.4. 2138-974 8-PF 21 200904946 The resulting green-emitting phosphor has an excitation band around a wavelength of 3 〇〇 to 4 〇〇 nm, and its emission peak is about 340 nm; for ultraviolet light-emitting diodes, The resulting green-emitting phosphor emits light efficiently, and its emission spectrum has an emission peak having a half width of about 103 nm, so that it has a broad emission peak. The excitation spectrum of this green-emitting phosphor is shown in Fig. 3, and its emission spectrum is shown in Fig. 4. Example 5: The fluorescent material of this example was obtained in the same manner as in Example 1, except that the raw materials used were different: 丨· 3164 g of calcium nitride, 1. 6500 g of oxygen 1匕矽, 〇·0709 g The vaporized hydrazine and 〇· 03 g of vaporized ammonium. The excitation spectrum and the emission spectrum of the fluorescent substance are measured, and the composition of the fluorescent substance is CauduuaShOuL. . The green fluorescent substance that is served has an excitation "▼ with a wavelength of 30 0~4〇〇nm, and its emission peak is about 330 nm; for the ultraviolet light diode, The luminescent light substance emits light efficiently, and the emission peak of the emitted light 4 has a half width of about 103 nm, so that it has a broad emission peak. The excitation spectrum of this green-emitting phosphor is shown in Fig. 3, and its emission spectrum is shown in Fig. 4. x Example 6 : The phosphor of this example was obtained in the same manner as in Example 1, except that the ruthenium was different: 1.4472 g of nitriding, "15" oxygen 8 〇〇g nitriding矽, 0.0780 g of gasification enthalpy and 0.03 g
2138-9748-pF 22 200904946 的：量測此螢光物質的激發光譜與發射光譜，此 爱九物貝的組成為Ca 2 9 7 Eu〇 〇3Si2 7〇3 4N3 ” 近的If綠光螢光物質具有在波長為300，°⑽附 二36〇nm;對於發紫外光二極體 °所侍之發綠光螢光物質有效率地發藍綠光，且並發 =譜^射峰具有約83⑽的半寬度，故其具有寬的發 、^毛綠光螢光物質之激發光譜顯示於第5圖，而1 發射光譜為第6W。 ㈡而其 例7 : 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同：14351 g的氮㈣、law g的氧 化石^、G.35GG g的氮化碎、〇.〇773 g的氯化銪與〇 〇3忌 的虱化錢。再量測此榮光物質的激發光譜與發射光譜，此 螢光物質的組成為Ca 2 9 7 EuQ Q3Si2 7〇3 9N3 Q。 9 所得之發綠光螢光物質具有在波長為3〇〇〜4〇〇⑽附 近的激發帶，其發射峰約為34〇nra;對於發紫外光二極體 而& ’所得之發綠光螢光物質有效率地發光，且其發射光 譜的發射峰具有約97⑽的半寬度，故其具有寬^發射 峰。此發綠光螢光物質之激發光譜顯示於第5圖，而其發 射光譜為第6圖。 例8 : 利用與例1相同的方式得到此例之螢光物質，但所使 2138-9748-PF 23 200904946 用的原料有所不同：1.4146 g的氮化鈣、1.4185 g的氧 化石夕、0.1380 g的氮化矽、0.0762 g的氣化銪與〇.〇3 g 的氯化銨。再量測此螢光物質的激發光譜與發射光譜，此 I 光* 物質的組成為 Ca2.97Eu〇.d3Si2.7〇4.8N2.4。 所得之發綠光螢光物質具有在波長為3〇(μ4〇〇 附 近的激發帶，其發射峰約為33〇 nm ;對於發紫外光二極體 而δ ’所得之發綠光螢光物質有效率地發黃綠光，且其發 射光。、s'的發射峰具有約1 〇 〇 nm的半寬度，故其具有寬的 發射峰。此發綠光螢光物質之激發光譜顯示於第5圖，而 其發射光譜為第6圖。 例9 : 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同：UK g的氮化飼、h⑽22 g的氧2138-9748-pF 22 200904946: Measure the excitation spectrum and emission spectrum of this fluorescent substance. The composition of this love nine-shell is Ca 2 9 7 Eu〇〇3Si2 7〇3 4N3 ” Near If Green Fluorescence The substance has a wavelength of 300, ° (10) attached to the second 36 〇 nm; for the ultraviolet light-emitting diodes, the green-emitting fluorescent material emits blue-green light efficiently, and the concurrent = spectral peak has about 83 (10) The half-width, so the excitation spectrum of the broad-emitting, green-green fluorescent substance is shown in Fig. 5, and the 1 emission spectrum is 6W. (2) and Example 7: The firefly of this example is obtained in the same manner as in Example 1. Light matter, but the raw materials used are different: 14351 g of nitrogen (four), law g of oxidized stone ^, G.35GG g of nitriding, 〇. 〇 773 g of lanthanum chloride and 〇〇 3 bogey 虱Re-measure the excitation and emission spectra of this luminescent material. The composition of this fluorescent material is Ca 2 9 7 EuQ Q3Si2 7〇3 9N3 Q. 9 The resulting green-emitting phosphor has a wavelength of 3〇. The excitation band near 〇4〇〇(10) has an emission peak of about 34〇nra; for the ultraviolet diode, & The substance emits light efficiently, and the emission peak of its emission spectrum has a half width of about 97 (10), so it has a broad emission peak. The excitation spectrum of the green-emitting phosphor is shown in Fig. 5, and its emission spectrum is Figure 6. Example 8: The phosphor of this example was obtained in the same manner as in Example 1, except that the raw materials used for 2138-9748-PF 23 200904946 were different: 1.4146 g of calcium nitride and 1.4185 g of oxidized stone. In the evening, 0.1380 g of tantalum nitride, 0.0762 g of gasified ruthenium and 〇.〇3 g of ammonium chloride. The excitation and emission spectra of the phosphor are measured, and the composition of the I light* material is Ca2. 97Eu〇.d3Si2.7〇4.8N2.4 The resulting green-emitting phosphor has an excitation band at a wavelength of 3 〇 (μ4〇〇, an emission peak of about 33 〇 nm; for ultraviolet light-emitting diodes) The green fluorescent material obtained by δ 'is yellowish green light efficiently and emits light. The emission peak of s' has a half width of about 1 〇〇 nm, so it has a broad emission peak. The excitation spectrum of the fluorescent substance is shown in Fig. 5, and the emission spectrum is shown in Fig. 6. Example 9: Utilization and Example 1 Same manner as the fluorescent material obtained in this Example, but the raw material to make different: UK g nitride feeding, h⑽22 g oxygen
^ 〇· 42 〇〇 g的氮化矽、0·0 82 9 δ的氣化銪與0.03 g :氣化銨。再量測此榮光物質的激發光譜與發射光譜，此 榮光物質的組成為Ca2.97Eu(».«3Si2.Α.ι.,。 所得之發綠光螢光物質具有在波長為3。〇~4〇。附 近的激發帶，其發射峰約為· nm;對於發紫外光二極體 :’所得之發綠光榮光物質有效率地發藍綠光 =料發射峰具有約6Gnffl的半寬度，故其具有寬的發 發射光營光物質之激發光譜顯示於第7圖，而其 I射光s晋為苐8圖。 2138-9748-PF 24 200904946 例ίο : 利用與例1相同的方式得到此例之螢光物質，但所使 用的原料有所不同·· U864 g的氮化飼、1.3G42 g的氧 化：、0: 1400 g的氮化矽、〇 〇8〇1 g的氯化銪與U3 g 的乳化叙。再量測此螢光物質的激發光譜與發射光譜，此 螢光物質的組成為Ca 2 9 7 Eu。。3以2 4〇44。 所得之發綠光營光物質具有在波長為_〜400 nm附 近的激發帶，其發射峰㈣34Gnm;對於發料光二極體 而言’所得之發綠光螢光物質有效率地發光，且直發射光 言晋的發射峰具有約1GG nm料寬度，故其具有寬的發射 峰。此發綠光螢光物質之激發光譜顯示於第7目，而其發 射光譜為第8圖。 例11 : 利用與例1相同的方式得到此例之螢光物質，作所使 用的原料有所不同：“759 g的氮化鈣、l 48〇〇 g的氧 化矽、0.0795 g的氣化銪與〇.03 2的氯化銨。再量測此 螢光物質的激發光譜與發射光譜，此螢光物質的組成為^ 〇· 42 〇〇 g of tantalum nitride, 0·0 82 9 δ gasification enthalpy and 0.03 g: vaporized ammonium. The excitation spectrum and the emission spectrum of the glory material are measured. The composition of the glory material is Ca2.97Eu(».«3Si2.Α.ι., and the resulting green light fluorescent material has a wavelength of 3. 〇~ 4〇. The vicinity of the excitation band, its emission peak is about · nm; for the UV diode: 'The resulting green glory material efficiently emits blue-green light = material emission peak has a half width of about 6Gnffl, so The excitation spectrum of the luminescence material having a broad emission light is shown in Fig. 7, and the I ray s is promoted as 苐8. 2138-9748-PF 24 200904946 Example ίο : This example is obtained in the same manner as in Example 1. Fluorescent material, but the raw materials used are different · U864 g nitride feed, 1.3G42 g oxidation: 0: 1400 g of tantalum nitride, 〇〇8〇1 g of tantalum chloride and U3 The emulsification of g. The excitation spectrum and the emission spectrum of the fluorescent substance are measured. The composition of the fluorescent substance is Ca 2 9 7 Eu. 3 is 2 4 〇 44. The obtained green light camping light substance has The excitation band near the wavelength of _~400 nm has an emission peak (four) of 34 Gnm; for the light-emitting diode, the resulting green-emitting phosphor has Efficiently emits light, and the emission peak of the direct-emitting optical ray has a width of about 1 GG nm, so it has a broad emission peak. The excitation spectrum of the green-emitting phosphor is shown in the seventh order, and its emission spectrum is 8 Fig. 11 : The phosphor of this example was obtained in the same manner as in Example 1 except that the raw materials used were different: "759 g of calcium nitride, 128 g of yttrium oxide, 0.0795 g of Gasification of cesium and 〇.03 2 ammonium chloride. The excitation spectrum and emission spectrum of the fluorescent substance are measured, and the composition of the fluorescent substance is
Ca2.97EU〇.〇3Si2.4〇4.8N2.0。 所得之發綠光螢光物質具有在波長為3〇〇〜4〇〇⑽附 近的激發帶，其發射峰約為340 nm;對於發紫外光二極體 而言，所得之發綠光勞光物質有效率地發光，且其發射光 譜的發射峰具有約100 的半寬度’故其具有寬的發射 峰。此發綠光螢光物質之激發光譜顯示於第7圖，而其發 2138-9748-PF 25 200904946 射光譜為第8圖。 所得之發綠光螢光物質的組成顯示於表1中，且X/ + a)與z/y之各值也顯示於表2中。 表1 螢光物質的組成式 例1 Ca8.97E110.03S1 8〇i〇Ni〇 例2 Ca2. 97EU0. 03S1 3〇3. 6N3. 6 例3 Ca2. 97EU0. 03S1 3〇4. 5N3. 0 例4 Ca2. 97EU0. 03S1 3〇5. 4N2. 4 例5 Ca2. 97Eu〇.03Si3〇6. 0N2. 0 例6 Ca2.97E110· tnSi 2.7O3.4N3.4 例7 Cd.2. 97EU0. 03S1 2. 7〇3. 9N3. 0 例8 Csi2 . 97EU0. 03S1 2. 7〇4. 8N2. 4 例9 C a 2 . 97E1I0. 03S i 2. 4〇3. 1 N3. 1 例10 Ca2. 97EU0. 03S1 2. 4〇4. 2N2. 4 例11 〇Ε2.9τΕΐΐ0.038Ϊ2.4〇4.δΝ2.0 表2 各組成元素的組成比例 W a X Y Z x/(w+a) z/y 例1 8.97 0.03 8.0 10 10 0.889 1. 0 例2 2.97 0.03 3.0 3.6 3.6 1.0 1.0 例3 2.97 0.03 3.0 4.5 3.0 1. 0 0. 667 例4 2.97 0.03 3.0 5.4 2.4 1.0 0.444 例5 2.97 0.03 3.0 6. 0 2.0 1.0 0.333 例6 2.97 0.03 2.7 3.4 3.4 0.9 1.0 例7 2.97 0.03 2.7 3. 9 3. 0 0.9 0. 769 例8 2. 97 0.03 2.7 4.8 2.4 0.9 0.5 例9 2. 97 0. 03 2.4 3. 1 3. 1 0.8 1.0 例10 2. 97 0. 03 2.4 4.2 2.4 0.8 0.571 例11 2.97 0.03 2.4 4.8 2. 0 0.8 0.417 26Ca2.97EU〇.〇3Si2.4〇4.8N2.0. The resulting green-emitting phosphor has an excitation band near a wavelength of 3 〇〇 4 〇〇 (10) and an emission peak of about 340 nm; for the ultraviolet light-emitting diode, the resulting green light-emitting material It emits light efficiently, and its emission spectrum has an emission peak with a half width of about 100' so that it has a broad emission peak. The excitation spectrum of this green-emitting phosphor is shown in Fig. 7, and its emission spectrum is 2138-9748-PF 25 200904946. The composition of the obtained green light-emitting fluorescent substance is shown in Table 1, and the values of X/+ a) and z/y are also shown in Table 2. Table 1 Composition of the fluorescent substance Example 1 Ca8.97E110.03S1 8〇i〇Ni〇Example 2 Ca2. 97EU0. 03S1 3〇3. 6N3. 6 Example 3 Ca2. 97EU0. 03S1 3〇4. 5N3. 0 Example 4 Ca2. 97EU0. 03S1 3〇5. 4N2. 4 Example 5 Ca2. 97Eu〇.03Si3〇6. 0N2. 0 Example 6 Ca2.97E110· tnSi 2.7O3.4N3.4 Example 7 Cd.2. 97EU0. 03S1 2 9〇3. 9N3. 0 Example 8 Csi2 . 97EU0. 03S1 2. 7〇4. 8N2. 4 Example 9 C a 2 . 97E1I0. 03S i 2. 4〇3. 1 N3. 1 Example 10 Ca2. 97EU0. 03S1 2. 4〇4. 2N2. 4 Example 11 〇Ε2.9τΕΐΐ0.038Ϊ2.4〇4.δΝ2.0 Table 2 Composition ratio of each component element W a XYZ x/(w+a) z/y Example 1 8.97 0.03 8.0 10 10 0.889 1. 0 Example 2 2.97 0.03 3.0 3.6 3.6 1.0 1.0 Example 3 2.97 0.03 3.0 4.5 3.0 1. 0 0. 667 Example 4 2.97 0.03 3.0 5.4 2.4 1.0 0.444 Example 5 2.97 0.03 3.0 6. 0 2.0 1.0 0.333 Example 6 2.97 0.03 2.7 3.4 3.4 0.9 1.0 Example 7 2.97 0.03 2.7 3. 9 3. 0 0.9 0. 769 Example 8 2. 97 0.03 2.7 4.8 2.4 0.9 0.5 Example 9 2. 97 0. 03 2.4 3. 1 3. 1 0.8 1.0 Example 10 2. 97 0. 03 2.4 4.2 2.4 0.8 0.571 Example 11 2.97 0.03 2.4 4.8 2. 0 0.8 0.417 26
2138-9748-PF 200904946 【圖式簡單說明】 第1圖係為實施例1之發綠光螢光物質的激發光譜； 第2圖係為實施例1之發綠光螢光物質的發射光譜； 第3圖係為實施例2到5之發綠光螢光物質的激發光 譜； 的發射光 第4圖係為實施例2到5之發綠光螢光物質 譜； 第5圖係為實施例6到8之發綠光螢光物質 的激發光 第6圖係為實施例6到8之笋终#， >、， <知綠先螢光物質的發射光 譜； 光譜； 第7圖係為實施例9到11 之發綠光螢光物質的激發 i. 第8圖係為實施例6到 譜；以及 之發綠光螢光物質的 第9圖係為本發明之發光裝置之— 示意圖 發射光 【主要元件符號說明】 101〜透明基材 102~螢光物質粉末 10 3〜透明樹脂體 105〜發光二極體 11卜發光裝置2138-9748-PF 200904946 [Simplified description of the drawings] Fig. 1 is an excitation spectrum of the green-emitting phosphor of Example 1, and Figure 2 is an emission spectrum of the green-emitting phosphor of Example 1. Figure 3 is an excitation spectrum of the green-emitting phosphors of Examples 2 to 5; Figure 4 of the emitted light is the green light-emitting material mass spectrum of Examples 2 to 5; Figure 5 is an example. The excitation light of the green light-emitting substance of 6 to 8 is the emission spectrum of the bamboo shoots of Examples 6 to 8, >, <the emission spectrum of the green fluorescent material; the spectrum; Excitation of the green-emitting phosphors of Examples 9 to 11 i. Figure 8 is a spectrum of Example 6; and Figure 9 of the green-emitting phosphor is a schematic of the light-emitting device of the present invention. Emission light [Description of main component symbols] 101~ Transparent substrate 102~ Luminescent substance powder 10 3~ Transparent resin body 105~ Light-emitting diode 11
2138-9748-PF2138-9748-PF
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| JP5515141B2 (en) * | 2009-03-16 | 2014-06-11 | Ｎｅｃライティング株式会社 | Phosphor and fluorescent lamp |
| JP5515142B2 (en) * | 2009-03-16 | 2014-06-11 | Ｎｅｃライティング株式会社 | Phosphor and fluorescent lamp |
| WO2011019191A2 (en) * | 2009-08-10 | 2011-02-17 | 엘지이노텍주식회사 | Phosphor, preparation method thereof, and white light emitting device |
| US9909058B2 (en) | 2009-09-02 | 2018-03-06 | Lg Innotek Co., Ltd. | Phosphor, phosphor manufacturing method, and white light emitting device |
| KR101163902B1 (en) | 2010-08-10 | 2012-07-09 | 엘지이노텍 주식회사 | Light emitting device |
| TWI456027B (en) * | 2010-03-03 | 2014-10-11 | Hitachi Ltd | Closed material sheet with wavelength conversion material and solar cell using the same |
| KR101441485B1 (en) * | 2013-09-17 | 2014-09-17 | 한국과학기술연구원 | Green-emitting upconversion nanophosphor and synthesis method thereof |
| JP2013256675A (en) * | 2013-10-02 | 2013-12-26 | Nec Lighting Ltd | Green emission oxynitride phosphor |
| TWI831680B (en) * | 2023-04-27 | 2024-02-01 | 隆達電子股份有限公司 | Light conversion material and light emitting device and display device including the same |
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| JP3609365B2 (en) * | 2001-10-19 | 2005-01-12 | 株式会社東芝 | Semiconductor light emitting device |
| EP1413618A1 (en) * | 2002-09-24 | 2004-04-28 | Osram Opto Semiconductors GmbH | Luminescent material, especially for LED application |
| WO2004036962A1 (en) * | 2002-10-14 | 2004-04-29 | Philips Intellectual Property & Standards Gmbh | Light-emitting device comprising an eu(ii)-activated phosphor |
| JP4466447B2 (en) * | 2002-10-16 | 2010-05-26 | 日亜化学工業株式会社 | Oxynitride phosphor |
| JP4415548B2 (en) * | 2002-10-16 | 2010-02-17 | 日亜化学工業株式会社 | Light emitting device using oxynitride phosphor |
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| EP2366754B1 (en) * | 2004-09-22 | 2014-08-27 | National Institute for Materials Science | Phosphor, production method thereof and light emitting instrument |
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| JP4798335B2 (en) * | 2004-12-20 | 2011-10-19 | Ｄｏｗａエレクトロニクス株式会社 | Phosphor and light source using phosphor |
| JP5145934B2 (en) * | 2005-03-04 | 2013-02-20 | 三菱化学株式会社 | Phosphor and method for producing the same, and light emitting device using the phosphor |
| KR100682874B1 (en) * | 2005-05-02 | 2007-02-15 | 삼성전기주식회사 | White light emitting device |
| JP4215046B2 (en) * | 2005-11-24 | 2009-01-28 | 日亜化学工業株式会社 | Nitride phosphor and light emitting device using the same |
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