TW201127938A - Co-doped silicooxynitrides - Google Patents

Co-doped silicooxynitrides Download PDF

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Publication number
TW201127938A
TW201127938A TW099122715A TW99122715A TW201127938A TW 201127938 A TW201127938 A TW 201127938A TW 099122715 A TW099122715 A TW 099122715A TW 99122715 A TW99122715 A TW 99122715A TW 201127938 A TW201127938 A TW 201127938A
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Taiwan
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cerium
composite
phosphor
lanthanum
light
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TW099122715A
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English (en)
Inventor
Holger Winkler
Ralf Petry
Tim Vosgroene
Thomas Juestel
Dominik Uhlich
Arturas Katelnikovas
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Merck Patent Gmbh
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Publication of TW201127938A publication Critical patent/TW201127938A/zh

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Description

201127938 六、發明說明： 【發明所屬之技術領域】 本發明係關於由6-3-6-4鹼土金屬矽氧氮化物組成之複合 物（其係與钍、釕、餓、氟及氣共摻雜），關於其製備，及 關於其作為磷光體之用途和關於用於暖白光LEd或所謂的 按需隨按需選色應用中之LED轉換磷光體。 【先前技術】 按需選色之概念係意指藉由使用一或多種磷光體之 PcLED(=磷光體轉換LED)產生具有特定色點之光。使用此 概念（例如）以製作某些公司（例如）用於闡明公司標誌、商 標等之設計。 爲藉由LED TV背光源獲得高色空間，需要深紅色磷光 體’其在620 nm至660 nm之範圍内具有一發射最大值。熟 習此項技術者已知之合適材料系統係矽氮化物及鋁矽氮化 物破光體（Xie，Sci, Technol. Adv. Mater. 2007, 8, 588-600): 1-1-2 氮化物’諸如（例如）CaSiN2:Eu2+(Le Toquin,
Cheetham’ Chem. Phys. Lett. 2006，423，352)，2-5-8氮化 物’諸如（Ca，Sr，Ba)2Si5N8:EU2+(Li 等人，Chem. Mater. 2005，15，4492)，及鋁矽氮化物，諸如（Ca，Sr)A1SiN3:Eu2+ (K. Uheda等人，Electrochem. Solid State Lett. 2006，9, H22)。 如以上提及之氮化物磷光體具有諸多缺點，其導致此等 材料無法大量獲得：特定言之，高純度要求代表工業界僅 可以更大努力方可滿足之挑戰。因此，極低之碳或氧濃度 148290.doc 201127938 導致碟光體之效率敏感地降低。但是，實際上無法避免氧 雜質’因為即使起始材料（諸如si^4)及金屬氮化物（鹼土 金屬氮化物、氮化销）皆無法取得無氧形式物。替代起始 材料（諸如金屬氫化物）對氧及水分十分敏感，意指氧亦= 由此等組分引入磷光體中。標準製備方法（諸如碳熱還原 及氮化）導致磷光體中之碳雜質，而使此磷光體進行灰 化’降低亮度。 石夕氧氮化物SqSLC^N4係首次由s〇hn等人，j〇urn 〇f
Electr. S〇c· 155(2)，J58-J61 (2008)進行描述。 【發明内容】 因此，本發明之目的係以使此等複合物獲得更大光效率 之方式改質以上提及之6-3-6-4鹼土金屬矽氧氮化物。 驚If地發現若與趾 ' 釕、餓、說及/或氣進行共推雜， 可滿足對經濟上重要地進—步增加紅色石夕氧氮化物破光體 (Ca，Sr，Ba)6Si3〇6N4:Eu之轉化效率的要求。 因此，本發明關於與銪摻雜之6_3_6_4鹼土金屬矽氧氮化 物類型之複合4勿’其額外包含來自钍、舒、餓、氟及/或 氯系列之共播雜劑。 「6-3-6-4鹼土金屬矽氧氮化物」意指組合物 M6Si3〇6N4:Euh ’其中M表示驗土金屬三戈複數個驗土金屬 之混合物。 較佳係式I複合物： (Ca,Sr5Ba)6.x(Si1.yMey)3(0J.2Ma2z)6N4：Eux ⑴ 其中 148290.doc 201127938
Me=Th、Ru及 /或 〇s Ma=F及/或 Cl x<0.5 y<l及 z<0.1。 X值較佳係等於0.003至〇·2，y值（其表示共摻雜劑Me之 原子濃度）較佳係等於〇 〇〇〇1至〇 2，及2值較佳係等於 〇_〇〇〇5 至0·03。更佳係 x=0.005 至 0.15 及/或 y = 0.00l 至 〇 02。 相較於彼等具有相同組成但無灶、釕、锇、氟及/或氣 等共摻雜劑者，根據本發明式〗複合物或磷光體之較大亮 度可以熟習此項技術者已知之理論解釋。此較大亮度係藉 由較尚晶格品質在鹵化物之存在下產生。該等鹵化物極可 月&使固相反應中離子必需克服以可佔據固體結構中所需晶 格位置之擴散障壁降低。重金屬Th、Ru或Os極可能經由 所謂重原子效應而使磷光體的吸收增加。 根據本發明複合物之粒度係在nrn及30 μπι之間，較佳 係在1 μιη及20 μπι之間，更佳係在2及丨5 μιη之間。 此外’本發明係關於一種可藉由固態擴散方法混合含有 氮化碎、銪及鈣及/或锶及/或鋇之起始材料與至少一種含 有处、餓、釕、氟化物及/或氣化物之共摻雜劑（其可視需 要包含來自鹼金屬或鹼土金屬齒複合物或硼酸鹽複合物等 系列之助熔劑），及隨後熱後處理獲得的複合物。 此外’本發明係關於一種用於製備經銪摻雜之6-3-6-4鹼 土金屬；Ε夕氧氮化物類型複合物之方法，其具有以下加工步 148290.doc 201127938 驟： a) 藉由與至少4種選自含有氮化矽、銪、鈣、锶、鋇、 敍、铷、锇、氟化物及/或氯化物之材料之起始材料 混合製備經含有钍、铷、餓、氟化物及/或氣化物之 材料共掺雜之摻雜EU之6-3-6-4鹼土金屬矽氧氮化物 複合物， b) 熱後處理經钍、铷、餓、氟化物及/或氯化物共摻雜 之複合物， c) 利用HC1溶液及KOH溶液清洗經熱後處理之複合物。 用於製備複合物之起始材料如以上提及係由氮化石夕 (Si3N4)、氫化鈣及氟化銪及至少一種含有Th、Ru、〇s、f 及Cl之共摻雜劑組成。除了較佳的氮化物、氫化物及氟化 物之外’合適的起始材料亦係其他無機及/或有機物質， 諸如氰胺、二氰胺、氰化物、草酸鹽、丙二酸鹽、富馬酸 鹽、碳酸鹽、擰檬酸鹽、抗壞血酸鹽及乙醯丙酮酸鹽。 以上提及之熱後處理（參見加工步驟…係在還原條件下 (例如）利用成形氣體（例如90/10)、純氫氣及/或於含或不含 以上提及之氛圍之氨氛圍中進行數小時。煆燒過程期間溫 度係在1000°c及1800°c之間，較佳係1400eC至1600。(：達數 小時（較佳係8小時）。 此外’較佳係將磷光體轉移至高壓燒結爐中並在4〇至7〇 bar及1400至1600°C之溫度下煆燒6至10小時。 此外，墙光體較佳係在真空中進行熱均壓。 另外，該等磷光體較佳係先經HC1且隨後經K〇H(其消除 148290.doc 201127938 非晶體SiOJ清洗。此清洗步驟較佳係增加發射強度及磷 光體之吸收》 藉由以上提及之方法，可能產生任意所需形狀之根據本 發明複合物或磷光體，諸如球形粒子、薄片及結構化材料 及陶竞。根據本發明，將此等形狀概述為術語「成形 體」。該成形體較佳係「填光體主體」。 因此，本發明另外關於一種包含根據本發明複合物之成 形體’其具有粗糙表面，該表面具有包含Si〇2、Ti〇2、 Ah〇3、ZnO、Zr〇2及/或ΙΑ或其混合氧化物之奈米顆粒 及/或包含含有或不含來自銪、锇、釕、鉦、氟及/或氣系 列之摻雜劑之根據本發明複合物之粒子。 在另一較佳實施例中，該成形主體在LED晶片之反面具 有結構化（例如錐形）表面（參見WO 2〇〇8/〇58619，Merck， 將其全部範圍以引用的方式併入本申請案之全文中）。此 可使磷光體盡可能耦合輸出較多光。 成形體上之結構化表面係藉由利用已結構化之合適材料 進行後續塗佈，或在後續步驟中藉由（光）微影方法、蝕刻 方法或藉由使用能量或材料束或機械力作用之書寫方法產 生。 在另一較佳實施例中，根據本發明成形體在LED晶片之 反面上具有粗糙表面，其具有包含si〇2、Ti〇2、、
Zn〇2、Zr〇2及/或Yah或此等材料之組合及/或包含含有或 不含來自Th、RU、0s、！7及/或C1系列之摻雜劑之具有式工 磷光體組合物之粒子的奈米顆粒。在此粗糙表面具有高達 148290.doc 201127938 數100 nm之粗糙度。經塗佈表面具有可降低或預防總體反 射且根據本發明磷光體可更佳地耦合輸出光之優點（參見 WO 2008/058619(Merck)，將其全部範圍以引用的方式併 入本申請案之全文中）。 此外’根據本發明成形體在面離晶片之表面上較佳具有 一匹配反射係數之層體’其可簡化磷光體所發射之初級輻 射及/或輕射之搞合輸出。 在另一較佳實施例中，該成形體具有一連續表面塗層， 其係由 Si〇2、Ti〇2、Al2〇3、Zn〇、Zr〇2 及 / 或 γ203 或其混 合氧化物及/或不含活化劑銪之式I複合物組成。此表面塗 層具有以下優點：合適的塗層材料之折射率刻度可使該折 射係數與環境相匹配。在此情況下，構光體表面之光散射 減少且大部分光可穿透磷光體並於該處被吸收及轉換。此 外’經匹配折射係數之表面塗層因總體内部反射減少而可 由磷光體能耦合輸出更多光。 此外，若需囊封磷光體，以連續層體較有利。為抵消磷 光體或其部分對周圍環境中之擴散水或其他材料之敏感 性，此可能係必要的。另一利用密閉殼層囊封之原因係實 際磷光體因晶片所產生的熱而熱去耦合。此熱導致磷光體 之螢光產率的降低並亦可影響螢光之顏色。最終，此類型 之塗層可藉由防止磷光體產生的晶格振動傳播至環境中而 增加碟光體之效率。 此外’成形體較佳具有多孔表面塗層，其係由si〇2、 Ti〇2 Al2〇3、ZnO ' Zr02及/或Y2〇3或其混合氧化物及/或 148290.doc 201127938 含有或不含來自Eu、Th、Ru、〇s、F及/C1系列之摻雜劑之 式1複合物組成。此等多孔塗層提供進一步降低單一層體 之折射係數之可能性。此類型之多孔塗層可藉由三種習知 方法，如WO 03/027015中所描述般製成，將其全部範圍以 引用的方式併入本申請案之全文中：玻璃之蝕刻（例如鈉 鈣玻璃（參見US 4019884))，多孔層體之應用及多孔層體與 触刻操作之組合。 在另一較佳實施例中，該成形體具有利於化學鍵結或物 理釔σ至％ i兄之官能基之表面，較佳係由環氧樹脂或聚石夕 氧樹脂組成。此等官能基可係（例如）經由酮基鍵結並可與 基於裱氧化物及/或聚矽氧之黏合劑成分形成鏈結之酯或 其他衍生物。此類型之表面具有利於磷光體均勻併入黏合 劑中之優點。此外，藉此可將該磷光體/黏合劑系統之流 變性質以及適用期調節至一特定程度。因此簡化混合物之 處理。若靜電相互作用經由電荷波動或部分電荷而在系統 之間發生作用，此時係使用術語物理性結合至環境。 由於應用於LED晶片之根據本發明磷光體層較佳係由聚 矽氧與均勻磷光體粒子之混合物組成，且該聚矽氧具有表 面張力，此磷光體層在微觀級上係不均勻或該層體之厚度 非完全不變。 另一較佳實施例之薄片形磷光體之製備係藉由習知方法 由相應金屬鹽及/或稀土鹽進行。該製備方法係詳細描述 於EP 763573及WO 2008/058620中，將其全部範圍以引用 的方式併入本申請案之全文中《可藉由水性分散液或懸浮 148290.doc 201127938 液之沉澱反應以磷光體層塗佈天然或合成製成的、高安定 性載體或基材包括（例如）雲母、Si〇2、Al2〇3、Zr〇2、破璃 或Τι〇2薄片（其具有極大寬高比，原子級光滑表面及可調 節厚度）的方式製備此等薄片形磷光體。除了雲母、 Zr02、Si02、Α12〇3、玻璃或Ti〇2或其混合物之外，該等薄 片亦可由磷光體材料本身組成或由一種材料構成。若該薄 片本身僅用作磷光體塗層之載體，後者需由可穿透LED之 初級輻射’或吸收初級輻射及將此能量轉移至磷光體層之 材料組成。薄片形磷光體係分散於樹脂（例如聚矽氧或環 氧樹脂）中，且此分散液係施用於led晶片。 可以大工業規模製備厚度為50 nm至約20 μιη，較佳係在 150 nm及5 μπι之間之薄片形磷光體。在此直徑係5〇 11爪至 20 μηι。通常其具有1:1至4〇〇:1且特定言之3:1至1〇〇:1之寬 南比（直徑對粒子厚度之比率）。薄片尺寸（長度X寬度）係取 决於配置β薄片亦適合作為轉換層内之散射中心，特定言 之若其等具有特別小之尺寸時。 面對LED晶片之根據本發明薄片形磷光體之表面可具有 一對於LED晶片發射之初級輻射之抗反射作用之塗層。此 導致初級輻射之回散射降低，可使後者更佳耦合至根據本 發明磷光體主體中。 適用於此目的係（例如）匹配折射係數之塗層，其需具有 以下厚度d:d=[LED晶片之初級輻射的波長/(4*磷光體陶瓷 之折射係數）]’參見（例如）Gerthsen，Physik [Physics]
SpHnger Verlag，第18版，1995。此塗層亦可由光子晶體組 148290.doc 201127938 成，其亦可包括薄片形鱗光體表面之結構化以達到特定6 能度。 呈陶瓷體形式之根據本發明成形體係以類似於w〇 2〇〇8/017353(Merck)所描述之方法製備，將其所有範圍以 引用的方式併入本申請案之全文中。在此方法中，藉由相 應起始材料與摻雜劑混合製備磷光體，隨後令其進行均壓 並以均勻、薄及無孔薄片形式或離晶片一段距離（遠離鱗 光體概念）直接施用於晶片表面上。各別配置尤其取半於 led裝置之構架，其中熟習此項技術者可選擇有利的配 置。因此磷光體之激發及發射無位置依賴性變化。其意指 隨其提供的LED發射顏色穩定之均勻光錐並具有高光輸 出。可以大工業規模製備陶瓷磷光體主體，如厚度為數 100 nm至約500 μιη之薄片。該薄片尺寸（長度χ寬度）係取 決於配置。在直接施用於晶片之情況中，該薄片之尺寸應 根據晶片尺寸(約100μΐΏ * 1〇〇μιη至若干_2)或合適晶片 配置（例如覆晶配置）相應地具有晶片表面之約1〇%至3〇% 之特定過大尺寸選擇^磷光體薄片係安裝在製成 上’所有射出的光錐穿過該薄片。 陶究磷光體主體之側表面可塗佈有輕質金屬或貴金屬， 1佳係1呂或銀。-該金屬塗層具有光不從磷光體主體側面射 之作用。側面射出的光可降 nt, ^ 降低LED耦合輸出之光電流。 间究磷光體主體之金屬塗居 如τ也 層係在均壓獲得條桿或薄後之 工步驟中進行，其中條浐 切害斗、’于或薄片可在金屬塗佈前視需要 成所尺寸。為此，f仏丨L11 (U如）利用包含硝酸銀及葡萄糠 148290.d〇c 201127938 之溶液潤濕側表面，並隨後使其在高溫下暴露於氨氛圍 中。銀塗層（例如）在此過程中形成於側表面上。 或者，無電流金屬化方法亦係合適，參見（例如） Hollemann-Wiberg, Lehrbuch der Anorganischen Chemie [Text-book of Inorganic Chemistry], Walter de Gruyter Verlag 或 Ullmanns Enzyklopadie der chemischen Technologie [Ullmann’s Encyclopaedia of Chemical Technology]。 若需要，可使用水-玻璃溶液使陶瓷磷光體主體固定於 LED晶片之底座。 在另一實施例中，陶瓷填光體主體在LED晶片之反面具 有結構化（例如錐形）表面。此可使磷光體主儘可能耦合輸 出較多之光。藉由使用具有結構化壓板之壓模進行均壓並 因此將結構壓印在表面上的方式在磷光體主體上製造結構 化表面。若目標係製造最薄的可能磷光體主體或薄片，則 需要結構化表面。壓樟條件係熟習此項技術者已知（參見j Kriegsmann, Technische keramische Werkstoffe [Technical Ceramic Materials],第 4 章，Deutscher Wirtschaftsdienst， 1998) 〇較重要係所使用的壓榨溫度係欲壓榨物質之熔點 的 2/3 至 5/6。 本發明另外關於一種用於製造成形體，較佳係磷光體主 體之方法’其具有以下加工步驟： a)藉由混合至少4種選自含有氮化矽、銪、鈣、锶、鋇、 釕、趾、餓、氟化物及/或氯化物之材料之起始材料製備 與含有钍、铷、锇、氟化物及/或氣化物之材料共摻雜之 148290.doc 201127938 摻雜銪之6-3-6-4之驗土金屬梦氧氮化物複合物， b) 熱後處理經灶、麵、餓、氟化物及/或氣化物共摻雜之 複合物並形成具有粗糙表面之成形體， c) 利用含有 Si02、Ti〇2、Al2〇3、ZnO、Zr02及 / 或 Y203 或 其混合氧化物之奈米顆粒或利用包含根據本發明複合物之 奈米顆粒塗佈表面。 此外，根據本發明磷光體之激發性係延伸至一寬廣範 圍，其係從約350 nm延伸至530 nm，較佳係430 nm至約 500 nm。因此，此等磷光體不僅適合以發射uv或藍光之 初級光源（諸如LED或習知放電燈（例如基於Hg))激發，亦 適用於在451 nm處利用藍色ιη3 +線之光源本身。 本發明另外關於一種具有至少一種發射最大值在25〇 nm 至530 nm之範圍内，較佳係350 nm至約5〇〇 nm之初級光源 之照明部件。特佳範圍係在44〇及48〇 nm之間，因為初級 幸W射係藉由根據本發明之複合物或鱗光體部分或完全轉變 為更長波長之輻射。此照明部件較佳係發射白光或發射具 有特疋色點之光（按需選色原理）。根據本發明照明部件之 較佳實施例係描述於圖5至1 6中。 在根據本發明照明部件之較佳實施例中，光源係發光的 氮化銦鋁鎵，特定言之具有式IniGajAlkN者，其中， ，（^k及i+j+k=l。此類型光源之可能形式係熟習此項技 術者已知。此等可係各種結構之發光led晶片。 在另一根據本發明照明部件之較佳實施例中，光源係基 於ZnO TCO(透明導電氧化物）、211以或Sic之發光配置或 148290.doc •14- 201127938 基於有機發光層（OLED)之配置。 在另-根據本發明照明部件之較佳實施例中，光源係— 顯示電致發光及/或光致發光之來源。該光源另外亦可係 電漿源或放電源。 根據本發明磷光體可分散於樹脂中（例如環氧樹脂或聚 矽氧樹脂）中或取決於應用，以既定合適的尺寸比率直接 配置在初級光源上或者遠離該處地配置（後者配置亦包含 「遠離磷光體技術」）。遠離磷光體技術之優點係熟習此 項技術者已知且（例如）由以下公開案顯示：Japanese J〇urn ofAppl. Phys.第 44卷，第 21 號（2〇〇5)，L649-L651。 在另一實施例中，照明部件中磷光體及初級光源間之光 耦合較佳係藉由光導配置獲得。因此初級光源可能安裝在 中心位置處並可視需要藉由光導裝置（諸如（例如）光纖）耦 合至磷光體。以此方式，可能獲得適於照明希望之光，其 僅係由一或多種可經配置形成光簾之磷光體及耦合至初級 光源之光波導組成。以此方式，可將強的初級光源放置在 有利於電氣设備之位置並將包含耗合至光波導之填光體之 光源無電氣佈線，但僅以放置光波導取代地安裝在任意所 需位置處，。 本發明另外關於一種根據本發明複合物及成形體作為磷 光體或磷光體主體之用途。 本發明另外關於一種根據本發明複合物用於部分或完全 轉換由發光二極體發射之藍光或近UV光之用途。 此外’較佳係根據本發明複合物用於將發射之藍光或近 148290.doc 15 201127938 uv光轉換為可見白光輻射之用途。此外，較佳係根據本 發明.複合物根據「按需選色」概念將初級輻射轉換為特定 色點之用途。 可單獨或以與以下為熟習此項技術者熟知之磷光體之混 合物形式利用根據本發明式I複合物：
Ba2Si04：Eu2+, BaSi205：Pb2+, BaxSri,.xF2:Eu2+, BaSrMgSi207：Eu2+,
BaTiP207, (Ba,Ti)2P2〇7：Ti, Ba3W06:U, BaY2F8Er3 + ,Yb+, Be2Si〇4:Mn ， B14GG3O12, CaAl2〇4:Ce , CflLa4〇7：Ce ,
CaAl2〇4：Eu2+, CaAl204：Mn2+, CaAl4〇7：Pb2+,Mn2+, CaAl204：Tb3+, Ca3Al2Si3〇i2：Ce3 + , Ca3Al2Si3Oi2:Ce3 +， Ca3Al2Si302:Eu2+，
Ca2B509Br:Eu2+，Ca2B509Cl:Eu2+，Ca2B509Cl:Pb2+, CaB204:Mn2+， Ca2B205:Mn2+，CaB204:Pb2+，CaB2P209:Eu2+，Ca5B2Si01():Eu3+，
Ca0.5Ba0.5Ali2〇i9:Ce3+,Mn2+，Ca2Ba3(P〇4)3Cl:Eu2+，CaBr2:Eu2+ 於 Si02 中，CaCl2:Eu2+於 Si02 中，CaCl2:Eu2+，Mn2+於 Si02 中， CaF2：Ce3+5 CaF2:Ce3+,Mn2+, CaF2:Ce3+,Tb3+, CaF2:Eu2+, CaF2：Mn2+, CaF2:U, CaGa2〇4：Mn2+, CaGa407:Mn2+, CaGa2S4:Ce3+, CaGa2S4:Eu2+, CaGa2S4:Mn2+，CaGa2S4:Pb2+, CaGe03:Mn2+，CaI2:Eu2+於 Si02 中，CaI2:Eu2+，Mn2+於Si02 中，CaLaB04:Eu3+，CaLaB307:Ce3+，Mn2+， Ca2La2B06.5:Pb2+, Ca2MgSi207, Ca2MgSi207：Ce3+, CaMgSi206:Eu2+, Ca3MgSi208:Eu2+，Ca2MgSi207:Eu2+，CaMgSi206:Eu2+，Mn2+， Ca2MgSi207:Eu2+,Mn2 +，CaMo04，CaMo04:Eu3 +，CaO:Bi3+， CaO:Cd2+，CaO:Cu+，CaO:Eu3 +，CaO:Eu3 +，Na+，CaO:Mn2+， CaO:Pb2+，CaO:Sb3+，CaO:Sm3+，CaO:Tb3+，CaO:Tl，CaO:Zn2+， Ca2P207:Ce3+，a-Ca3(P04)2:Ce3+，P-Ca3(P04)2:Ce3+，Ca5(P04)3Cl:Eu2+， 148290.doc 16 201127938
Ca5(P04)3Cl:Mn2+，Ca5(P04)3Cl:Sb3 +，Ca5(P04)3Cl:Sn2+，P-Ca3(P04)2:Eu2+，Mn2+, Ca5(P04)3F:Mn2+，Cas(P04)3F:Sb3+, Cas(P04)3F:Sn2+， a-Ca3(P04)2:Eu2+，p-Ca3(P04)2:Eu2+，Ca2P207:Eu2+，Ca2P207:Eu2+，Mn2+， CaP206:Mn2+，a-Ca3(P04)2:Pb2+，a-Ca3(P04)2:Sn2+，P-Ca3(P04)2:Sn2+， P-Ca2P2〇7：Sn,Mn, a-Ca3(P04)2：Tr, CaS:Bi3+, CaS:Bi3+,Na, CaS:Ce3+, CaS:Eu2+, CaS:Cu+,Na+, CaS:La3+, CaS:Mn2+, CaS04:Bi, CaS04：Ce3+, CaS04:Ce3+,Mn2+, CaS04：Eu2+, CaS04：Eu2+,Mn2+, CaS04：Pb2+, CaS:Pb2+, CaS:Pb2+,Cl, CaS:Pb2+,Mn2+, CaS:Pr3+,Pb2+,Cl, CaS:Sb3 + , CaS:Sb3 + ,Na, CaS:Sm3 + , CaS:Sn2+, CaS:Sn2+,F, CaS:Tb3 + , CaS:Tb3 + ,Cl, CaS:Y3 + , CaS:Yb2+, CaS:Yb2+,Cl, CaSi03：Ce3+, Ca3Si04Cl2:Eu2+s Ca3Si04Cl2：Pb2+, CaSi03：Eu2+, CaSi03：Mn2+5Pb, CaSi03：Pb2+, CaSi03:Pb2+,Mn2+, CaSi03:Ti4+, CaSr2(P04)2：Bi3+5 P-(Ca5Sr)3(P04)2：Sn2+Mn2+, CaTi〇.9Al〇.103:Bi3+, CaTi03:Eu3+，CaTi03:Pr3+, Ca5(V04)3Cl, CaW04, CaW04:Pb2+， CaW04：W, Ca3W06：U, CaYA104:Eu3+5 CaYB04:Bi3+, CaYB04：Eu3+, CaYB〇.8〇3-7：Eu3+, CaY2Zr06:Eu3+, (Ca,Zn,Mg)3(P04)2：Sn, CeF3, (Ce，Mg)BaAl丨丨O丨8:Ce，（Ce，Mg)SrAl"0丨8:Ce，CeMgAluOaCeiTb， Cd2B6〇ii：Mn2+, CdS:Ag+,Cr, CdS:In, CdS:In, CdS:In,Te, CdS:Te，CdW04, CsF，Csl, CsI:Na+，CsI:Tl, (ErCl3)0 25(BaCl2)0_75, GaN:Zn, Gd3Ga5012:Cr3 + , Gd3Ga5〇,2：Cr,Ce, GdNb04：Bi3 + , Gd202S:Eu3+, Gd202Pr3+, Gd202S:Pr,Ce5F, Gd202S:Tb3+, Gd2Si05:Ce3+, KA1"017:T1+，KGan017:Mn2+，K2La2Ti3O10:Eu，KMgF3:Eu2+, KMgF3：Mn2+, K2SiF6:Mn4+, LaAl3B40,2：Eu3+, LaAlB206：Eu3+, LaAl〇3：Eu3+, LaA103:Sm3+, LaAs04:Eu3+, LaBr3:Ce3+, LaB03:Eu3+, 148290.doc •17· 201127938 (La，Ce，Tb)P04:Ce:Tb，LaCl3:Ce3 +，La203:Bi3 +，LaOBr:Tb3+， LaOBr:Tm3+，：LaOCl:Bi3+，LaOCl:Eu3+，LaOF:Eu3+，La203:Eu3+， La203:Pr3+，La202S:Tb3+，LaP04:Ce3+，LaP04:Eu3+，LaSi03Cl:Ce3+， LaSi03Cl:Ce3+，Tb3+，LaV04:Eu3+，La2W3012:Eu3+，LiAlF4:Mn2+， LiAl508:Fe3 +，LiA102:Fe3 + , LiA102:Mn2+，LiAl508:Mn2+，
Li2CaP2〇7：Ce3+,Mn2+, LiCeBa4Si4〇i4：Mn2+, LiCeSrBa3Si4〇i4:Mn2+, LiIn〇2：Eu3 + , LiIn02:Sm3+, LiLa02：Eu3+, LuA103:Ce3+, (Lu,Gd)2Si05：Ce3+, Lu2Si05：Ce3+, Lu2Si2〇7：Ce3+, LuTa04:Nb5+, Lui.xYxA103：Ce3+, MgAl2〇4：Mn2+, MgSrAli〇〇i7:Ce, MgB2〇4：Mn2+, MgBa2(P〇4)2.§n2+，MgBa2(P04)2:U，MgBaP2〇7:Eu2+，MgBaP207:Eu2+，Mn2+， MgBa3Si2〇8-'Eu2+, MgBa(S04)2:Eu2+，Mg3Ca3(P04)4:Eu2+， MgCaP207:Mn2+，Mg2Ca(S04)3:Eu2+, Mg2Ca(S04)3:Eu2+，Mn2, MgCeAln〇i9：Tb3+, Mg4(F)Ge06:Mn2+, Mg4(F)(Ge,Sn)06:Mn2+, MgF2：Mn2+, MgGa2〇4：Mn2+, Mg8Ge2〇nF2：Mn4+, MgS:Eu2+, MgSi03:Mn2 +，Mg2Si04:Mn2+，Mg3Si03F4:Ti4+，MgS04:Eu2 + , MgS04：Pb2+, MgSrBa2Si2〇7：Eu2+, MgSrP207:Eu2+5 MgSr5(P04)4：Sn2+, MgSr3Si2〇8：Eu2+,Mn2+, Mg2Sr(S04)3：Eu2+, Mg2Ti04:Mn4+, MgW04, MgYB04：Eu3+, Na3Ce(P04)2：Tb3+, NaI:Tl, Na1.23K〇.42Eu〇.12TiSi4〇1i：Eu3+J Nai.23K〇.42Eu〇.i2TiSi5〇i3*xH2〇：Eu3 , Nai.29K〇,46Er〇,〇8TiSi4〇i 1 :Eu3 , Na2Mg3Al2Si2〇i〇：Tb, Na(Mg2-xMnx)LiSi4〇i〇F2：Mn, NaYF4：Er3+, Yb3+, NaY02:Eu3+, P46(70%)+P47(30°/〇), SrAl12019：Ce3+, Mn2+, SrAl2〇4：Eu2+, SrAl4〇7：Eu3+, SrAli2〇i9：Eu2+, SrAl2S4:Eu2+, Sr2B509Cl:Eu2+，SrB407:Eu2+(F，Cl,Br)，SrB407:Pb2+, SrB407:Pb2+, Mn2+, SrB8〇i3：Sm2+, SrxBayCl2Al2〇4-z/2：Mn2+, Ce3+, SrBaSi04：Eu2+, 148290.doc • 18 · 201127938
Sr(Cl，Br，I)2:Eu2+於 Si02 中，SrCl2:Eu2+於 Si02 中，Sr5Cl(P04)3:Eu， SrwFxB406.5:Eu2+, SrwFxByOz:Eu2+,Sm2+, SrF2:Eu2+, SrGa12〇i9：Mn2+, SrGa2S4:Ce3 +，SrGa2S4:Eu2+，SrGa2S4：Pb2+s SrIn204:Pr3 +， Al3 +，（Sr，Mg)3(P〇4)2:Sn，SrMgSi206:Eu2+，Sr2MgSi207:Eu2+, Sr3MgSi2〇8：Eu2+, SrMo04:U5 Sr0-3B203:Eu2+5Cl, p-Sr0-3B203:Pb2+, p-Sr0-3B203:Pb2+sMn2+, a-Sr0-3B203: Sm2+, Sr6P5BO20：Eu, Sr5(P04)3Cl:Eu2+, Sr5(P04)3Cl:Eu2+,Pr3 + , Sr5(P04)3Cl:Mn2+, Sr5(P04)3Cl:Sb3+, Sr2P207:Eu2+, p-Sr3(P04)2:Eu2+，Sr5(P04)3F:Mn2+， Sr5(P04)3F:Sb3+5 Sr5(P04)3F:Sb3+,Mn2+, Sr5(P04)3F:Sn2+, Sr2P207:Sn2+, P-Sr3(P04)2：Sn2+, p-Sr3(P04)2：Sn2+,Mn2+(Al), SrS:Ce3+, SrS:Eu2+, SrS:Mn2+, SrS:Cu+,Na, SrS04：Bi, SrS04：Ce3 + , SrS04:Eu2+, SrS04:Eu2+,Mn2+, Sr5Si4〇i〇Cl6:Eu2+, Sr2Si04:Eu2+, SrTi03:Pr3+, SrTi03:Pr3+,Al3+, Sr3W06:U, SrY203：Eu3+, Th02:Eu3+, Th02:Pr3+, Th02:Tb3+, YAl3B40,2：Bi3+, YAl3B40,2：Ce3+, YAl3B40,2：Ce3+,Mn, YAl3B4〇i2：Ce3+,Tb3+, YA13B4〇i2：Eu3+, YAl3B4〇i2：Eu3+,Cr3+, YAl3B4〇i2：Th4+,Ce3+,Mn2+5 YA103:Ce3+, Y3Al5012:Ce3+, Y3Al5012：Cr3+, YA103:Eu3+, Y3Al5〇i2：Eu3r, Y4A1209:Eu3+, Y3Al5012：Mn4+, YA103:Sm3+, YA103:Tb3+, Y3Al5〇i2：Tb3+, YAs04：Eu3+, YB03:Ce3+, YB03:Eu3+, YF3：Er3+,Yb3+, YF3:Mn2+, YF3：Mn2+,Th4+, YF3:Tm3+,Yb3+, (Y,Gd)B03:Eu, (Y,Gd)B03:Tb, (Y,Gd)203:Eu3+, Y1.34Gd〇.6〇03(Eu,Pr), Y2〇3：Bi3+, YOBr:Eu3+, Y203：Ce, Y203:Er3+, Y203：Eu3+(Y0E), Y203：Ce3+,Tb3+, YOCl:Ce3+, YOC1:Eu3+, YOF:Eu3+, YOF:Tb3+, Y203：Ho3+, Y202S:Eu3+, Y202S:Pr3+, Y202S:Tb3+, Y203:Tb3+, YP04：Ce3 + , YP04:Ce3+,Tb3+, YP04:Eu3 + , YP04：Mn2+,Th4+, 148290.doc •19· 201127938 YP〇4：V5 + , Y(P,V)〇4：Eu, Y2Si〇5：Ce3 + , YTa04, YTa04：Nb5+, YV04:Dy3+, YV04:Eu3+, ZnAl2〇4：Mn2+, ZnB204：Mn2+, ZnBa2S3：Mn2+, (Zn,Be)2Si〇4：Mn2+, Zn〇.4Cd〇.6S:Ag, Zn〇.6Cd〇.4S:Ag, (Zn,Cd)S:Ag,Cl, (Zn,Cd)S:Cu, ZnF2：Mn2+, ZnGa204, ZnGa2〇4：Mn2+, ZnGa2S4：Mn2+5 Zn2Ge04:Mn2+，（Zn，Mg)F2:Mn2+，ZnMg2(P04)2:Mn2+，(Zn，Mg)3(P04)2:Mn2+, ZnO:Al3 + ,Ga3 + , ZnO:Bi3 + , ZnO:Ga3 + , ZnO:Ga, ZnO-CdO:Ga, ZnO: S, ZnO:Se, ZnO.Zn, ZnS: Ag+,C1', ZnS: Ag,Cu,Cl, ZnS:Ag,Ni, ZnS:Au,In, ZnS-CdS(25-75), ZnS-CdS(50-50), ZnS-CdS(75-25), ZnS-CdS:Ag,Br,Ni, ZnS-CdS:Ag+,C1, ZnS-CdS:Cu,Br, ZnS-CdS:Cu,I, ZnS:Cr, ZnS:Eu2+, ZnS:Cu, ZnS:Cu+,Al3+, ZnS:Cu+,Cr, ZnS:Cu,Sn, ZnS:Eu2+, ZnS:Mn2+, ZnS:Mn,Cu, ZnS:Mn2+,Te2+, ZnS:P, ZnS:P3',Cl*, ZnS:Pb2+, ZnS:Pb2+,Cl', ZnS:Pb,Cu, Zn3(P04)2:Mn2+, Zn2Si〇4：Mn2+, Zn2Si〇4：Mn2+,As5+, Zn2Si04:Mn，Sb202，Zn2Si04:Mn2+，P，Zn2Si04:Ti4+，ZnS:Sn2+, ZnS:Sn,Ag，ZnS:Sn2+，Li+，ZnS:Te，Mn，ZnS-ZnTe:Mn2+，ZnSe:Cu+，Cl， ZnW04。 【實施方式】 將參照許多工作實例將本發明更詳細解釋於下。 以下實例係意圖闡述本發明。但是，不應將此等視為限 制。組合物中可使用的所有複合物或組分係已知及商業購 得或可藉由已知方法合成得到。實例中顯示的溫度通常係 以°C計。此外，不言而喻在描述及實例兩者中之組合物中 所添加的組分量通常加起來總和為100%。所提供的數據 百分率通常與既定關聯有關。但是，其等通常係與所表示 148290.doc -20- 201127938 之分量或總量之重量有關。 實例 實例 1 :製備5 g 81*5.94£|1。.。68丨3061\4 使6.8112§81^2〇4(入价人63&11，95%)、0.0689 §£112〇3 (Treibacher’99.99%；^0.9159ga-Si3N4(UBE，99%)S_ 瑙研缽中充滿乾燥N2之手套箱中彼此充分結合。將以此方 式獲得的粗製物質混合物轉移至襯有Mo箔片之a12〇3舟皿 内。在1200至1600°C及NVHVNH3氛圍下加熱該混合物達8 小時。 實例2 :製備5 g Sr5.94Euu6Si3O5.88N4F0.24 使 6.6736 g SrC204(Alfa Aesar，95%)、0.0689 g Eu2〇3 (Treibacher ’ 99.99%)、0.0984 g SrF2(Aldrich，99.998%)及 0.91 59 g ot-Si3N4(UBE ’ 99%)在瑪蹈研体中充滿乾燥n2之 手套箱中彼此充分結合。將以此方式獲得的粗製物質混合 物轉移至襯有Mo箔片之八丨2〇3舟m内。在12〇〇至i600°C及 N2/H2/NH3氛圍下加熱該混合物達8小時。 實例3 :製備5 g Srs.94Eu〇.06Si305.88N4Cl0.24 使 6.6168 g SrC204(Alfa Aesar ’ 95%)、0.0683 g Eu203 (Treibacher > 99.99%) > 0.1231 g SrCl2(Alfa Aesar > 99.5%) 及 0.9081 gα-Si3N4(UBE，99%)於瑪瑙研缽中充滿乾燥N2 之手套箱中彼此充分結合。將以此方式獲得的粗製物質混 合物轉移至概有Mof|片之Al2〇3舟皿内。在1200至1600°C 及N2/H2/NH3氛圍下加熱該混合物達8小時。 實例 4 ·製備 5 g Sr5.82Th〇.G6Eu〇.〇6Si3〇6N4 348290.doc •21 · 201127938 使 6.6444 g SrC2〇4(Alfa Aesar，95%)、0.0686 g Eu2〇3 (Treibacher，99.99%)、0.1030 g Th〇2(Merck，99%)及0.9119 g a-Si3N4(UBE，99%)於瑪瑙研缽中充滿乾燥n2之手套箱中 彼此充分結合。將以此方式獲得的粗製物質混合物轉移至 概有Mo猪片之AI2O3舟皿内。在1200至1600°C及N2/H2/NH3 氛圍下加熱該混合物達8小時。 實例 5 :製備5 g 81*5.82〇8。.。6£|10.。6813〇6]\4 使 6.6658 g SrC2〇4(Alfa Aesar，95%)、0.0688 g Eu203 (Treibacher，99.99%)、0.0869 g 0s02(Alfa Aesar，Os 83% min)及0.9148 g a-Si3N4(UBE，99%)於瑪瑙研缽中充滿乾燥 N2之手套箱中彼此充分結合。將以此方式獲得的粗製物質 混合物轉移至概有Mo箱片之AI2O3舟皿内。在1200至1600 °C及Νζ/ΗνΝΗ3氛圍下加熱該混合物達8小時。 實例 6 :製備 5 g SrswRiiueEiiowShOeP^ 使 6.7129 g SrC204(A】fa Aesar，95%)、0.0693 g Eu203 (Treibacher * 99.99%) > 0.0524 g Ru02(Alfa Aesar > 99.9%) 及0.9213 g cx-Si3N4(UBE，99%)於瑪瑙研缽中充滿乾燥^ 之手套箱中彼此充分結合。將以此方式獲得的粗製物質混 合物轉移至襯有Mo箔片之Aha舟皿内。在12〇〇至16〇〇t 及N2/H2/NH3氛圍下加熱該混合物達8小時。 實例7:高壓燒結實例1至6之磷光體 在各情況中，將5 g實例1至6之複合物置κΜ〇坩堝中並 轉移至南壓燒結爐中。將其中樣品在4〇至7〇匕紅之氮氣壓 力下以5至】0 K/min之升溫變率加熱至14〇〇至16〇〇。〇之溫 148290.doc •22· 201127938 度。該保持時間係6至1〇小時。 實例8.熱均壓實例1至6之碌光體 在各凊况中，將5 g實例1至6之複合物轉移至均壓熱壓 機中。該熱屋機係置於真空下，並將溫度升高至2〇〇。〔。 隨後以5至10 K/min將溫度升高至14〇〇至16〇〇。〇 ’並同時 將壓力值調至介於5G及細MPa間之值。保持時間係6至1〇 小時。 貫例9 .清洗實例1至8之鱗光體 在各情況中，將5 g實例1至8之複合物懸浮於1〇〇⑹之工 莫耳鹽酸中並在室溫下攪拌3小時。隨後利用抽氣濾出殘 留物並利用去離子水清洗直至中性。然後將經清洗的殘留 物懸浮於100…之丨莫耳K〇H溶液中並另外攪拌3〇分鐘。 隨後利用抽氣濾出殘留物並再次利用去離子水清洗直至中 性。 表1 . Srs.^Euo.MSisOeN4(作為參照）及根據本發明共摻雜磷 光體之光學性質 組合物 發射最大值『nml CIE 1931 χ,ν Sr5.94Eu〇.〇6Si3〇6N4 624 0.623 0.376 Sr5.94EU0.06Si3O5.88N4F0.24 623 0.622 0.377 Sr5.94ElI0.06Si3O5.88N4Cl0.24 625 0.625 0.374 Sr5.94Ru〇 〇6Eu〇.〇6Si3〇6N4 624 0.623 0.376 Sr5.94Th〇.〇6Eu〇.〇6Si3〇6N4 625 0.621 0.378 148290.doc •23- 201127938 【圖式簡單說明】 圖1 :顯示InGaN型之COB(板上連接式晶片）封裝，其係 用作白光之光源（LED)(1 =半導體晶片；2，3 =電接線；4= 轉換磷光體；7=板）。該磷光體係分佈於黏合劑透鏡中， 其同時代表二級光學元件並影響作為透鏡之光發射特性。 圖2 :顯示InGaN型之COB(板上連接式晶片）封裝，其係 用作白光之光源（LED)(1 =半導體晶片；2，3=電接線；4= 轉換磷光體；7=板）。該磷光體係直接位於分佈於薄黏合 劑層體中之LED晶片上。由透明材料組成之二級光學元件 可置於其上。 圖3 :顯示Golden Dragon®封裝’其係用於作為白光之 光源（LED)(1 =半導體晶片；2，3 =電接線；4=具有反射體 之空腔中的轉換磷光體）。該轉換磷光體係分散於黏合劑 中且該混合物充滿空穴。 圖4 :顯示SMD(表面安裝裝置）封裝，其中1 =外殼；2， 3 =電接線；4=轉換磷光體。該半導體晶片係藉由根據本發 明磷光體完全覆蓋。該SMD設計具有小型設計且因此適用 於習知照明之優點。 圖5:顯示發光二極體之圖示，其中1 =半導體晶片· 2， 3 =電接線；4 =轉換磷光體；5 =連接線，其中如黏合劑之頂 部球體般施用該磷光體。此形式之磷光體/黏合劑層體可 用作二級光學元件並影響（例如）光傳播。 圖6 .顯不發光二極體之圖示，其中1 =半導體晶片；2， 3 =電接線；4=轉換鱗光體；5 =連接線，其中如分散於黏合 148290.doc 24. 201127938 劑中之薄膜層體般施用該磷光體。另一用作二級光學元件 之組件諸如（例如）透鏡可容易地施用於此層體。 圖7 :顯示另一應用實例，其基本上已由US-Β 6,700,322 中已知°根據本發明磷光體係在此係與〇LED —起使用。 光源係有機發光二極體3〗，其係由實際有機薄膜3〇及透明 基板32組成。特定言之，薄膜3〇發射藍色初級光，其（例 如）係藉由PVK:PBD:香豆素（PVK為聚（η-乙烯基咔唑）之縮 寫；PBD為2-(4-聯苯基）_5-(4_第三丁基-苯基）_丨，3,4_噁二 唾之縮寫）產生。該發射藉由板據本發明磷光體之層體33 所形成之頂層部分轉換為黃色、二次發射光，經由初次及 一-人發射光之顏色混合整個導致發射白光。〇LED基本上 係由兩電極之間至少一層發光聚合物或所謂小分子組成， V、中α亥電極係由本身已知作為陽極之材料諸如（例 如）ΙΤΟ(氧化銦錫之縮寫）及作為陰極之高反應性金屬諸如 (例如）Ba或Ca組成之。在電極之間通常亦使用複數個層 體’其係用洞傳遞層或在Μ子區域内亦作力電子傳 遞層。所使用的發射聚合物係（例如）聚第類或聚螺材料。 【主要元件符號說明】 1 半導體晶片/外殼 2 電接線 3 電接線 4 轉換磷光體 5 連接線 7 板 I48290.doc _ 201127938 30 有機薄膜 31 有機發光二極體 32 透明基板 33 層體 148290.doc •26

Claims (1)

  1. 201127938 七、申請專利範圍： 1. 一種經銪摻雜之6-3-6-4驗土金屬矽氧氮化物類型之複合 物’其額外包含來自Th、Ru、Os、F及/或C1系列之共摻 雜劑。 2.如請求項1之複合物，其特徵在於式I: (Ca,Sr,Ba)6.x(Si1.yMey)3(01.zMa2z)6N4：Eux ⑴ 其中 Me=Th、RU及 /或 Os Ma=F及/或 Cl x<0.5 y<l及 z<0.1 〇 3·如請求項1或2之複合物，其特徵在於χ=〇 〇〇3至〇 2， y=0.000l 至 0.2及 Ζ=0·0005 至 0.03。 4·如請求項1或2之複合物，其特徵在於χ=〇〇〇5至〇 ΐ5及/ 或y=〇.〇oi至〇.〇2。 5.如請求項1或2之複合物，其藉由固態擴散方法使含有氮 化矽、銪及鈣及/或鰓及/或鋇之起始材料與至少一種之 含有鉉、锇、釕、氟化物及/或氯化物之共摻雜劑混合及 隨後熱後處理的方式獲得。 6· -種用於製備如請求項⑴項中任一項之複合物之方 法，其具有以下加工步驟： a)藉由混合至少4種選自含有氮化 銪、鈣、鳃、 貝、1土、釕、锇、氣化物及/或氯化物之材料之起始材料 148290.doc 201127938 製備掺雜銪之6-3-6-4鹼土金屬矽氧氮化物，其係經含有 钍、釕、餓、氟化物及/或氯化物之材料共摻雜， b) 熱後處理經钍、釕、锇、氟化物及/或氣化物共摻雜 之複合物， c) 利用HC1溶液及KOH溶液清洗經熱後處理之複合物。 7. —種包含如請求項】至5項中任一項之複合物之成形體， 其特徵在於其具有粗糙表面，該表面具有包含Si〇2、 Ti〇2、Al2〇3、Zn0、Zr〇2及/或丫2〇3或其混合氧化物之 奈米顆粒及/或包含含有或不含來自銪、钍、釕、餓、氟 及/或氣系列之摻雜劑之如請求項丨至5項中任一項之複合 物的粒子。 8. —種包含如請求項i至5項中任一項之複合物之成形體， /、特徵在於其具有連續表面塗層，該塗層係由、 Τι〇2、Al2〇3、Zn〇、Zr〇2&/或γ2〇3或其混合氧化物及/ 或不含活化劑銪之如請求項1至5項中任一項之複合物組 9. 一種包含如請求項丨至5項中任一項之複合物之成形體， 其特徵在於其具有多孔表面塗層，該塗層係由Si02、 Ti〇2、Al2〇3、ZnO、心〇2及/或γ2〇3或其混合氧化物及/ 或’含有或不含來自銪、敍、釕、锇、敗及/或氣系列之摻 雜劑之如請求項丨至5項中任一項之複合物組成。 10. 種包含如請求項1至5項中任一項之複合物之成形體， 其特徵在於該表面具有有助於化學鍵結或物理結合至環 铤，較佳係由環氧樹脂或聚矽氧樹脂組成之環境之官能 148290.doc 201127938 基。 π. —種用於製備如請求項8至10項中任—項之成形體之方 法，其具有以下加工步驟： a) 藉由混合至少4種選自含有氮化矽、銪、鈣、鋇、 鋇、钍、釕、餓、氟及/或氯之材料之起始材料製備摻雜 銪之6-3-6-4鹼土金屬矽氧氮化物複合物，其係經含有 灶、釕、锇、氟化物及/或氣化物之材料共摻雜， b) 熱後處理經钍、釕、餓、氟及/或氣共摻雜之複合 物， c) 利用包含 Si02、Ti〇2、Al2〇3、Zn〇、心〇2及 /或 γ2〇3 或其混合氧化物之奈米顆粒或利用包含含有或不含摻雜 劑之如請求項1至5項中任一項之複合物之奈米顆粒塗佈 表面。 12. 如清求項11之方法，其特徵在於加工步驟b)之後係接著 進行利用HC1溶液及KOH溶液之清洗步驟。 13. —種照明部件，其具有至少一種發射最大值在25〇 nm至 530 nm之範圍内，較佳係在35〇 1^及5〇〇 nm之間之初級 光源’其中此輻射係藉由如請求項i至5及7至1 〇中任一 項之複合物及/或磷光體主體部分地或完全轉換為較長波 長之輻射。 14. 如請求項13之照明部件，其特徵為該光源係發光的氮化 銦鋁鎵，特定言之具有式IniGajAlkN者，其中，〇匀， 0$k及 i+j + k=l。 15_如請求項13之照明部件’其特徵在於該光源係基於 148290.doc 201127938 ZnO、TCO(透明導Φ条儿此、 守電氣化物）、ZnSe或SiC之發光複合 物。 16.如請求項13之照明A _ 件，其特徵在於該光源係基於有機 發光層體之材料。 17 ·如請求項13之昭明ar从 # ”，、月。卩件’其特徵在於該光源係電漿燈或 放電燈。 18. 如咕求項13至17項中任一項之照明部件，其特徵在於該 鱗光體係直接配置於初級光源上及/或遠離該處。 19. 如請求項13至17項中乜 _g ^ 〇 $甲任一項之照明部件，其特徵在於磷 光體及初級光源間之井巍人 心尤麵合係猎由光導配置方式獲得。 20. —種至少一種如請龙担 項1至5項中任一項之複合物作為磷 光體之用途。 21\種至少一種如請求項1至5項中任-項之複合物之用 ，、係作為用於。卩分或完全轉換由發光三極體發射之 藍光或近UV光之轉換磷光體。 22· 一種至少一種如請求項1至5項中任-項之複合物之用 途，其係作為根據”選色概念將初 色點之轉換磷光體。 -挟為特疋 23. —種如請求項^ 體之用途。 $中任一項之成形體作為磷光體主 148290.doc
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