TWI421328B - 螢光材料與白光發光裝置 - Google Patents
螢光材料與白光發光裝置 Download PDFInfo
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- 239000000463 material Substances 0.000 claims description 41
- 239000000126 substance Substances 0.000 claims description 14
- 238000000295 emission spectrum Methods 0.000 claims description 13
- 229910052775 Thulium Inorganic materials 0.000 claims description 12
- 230000005284 excitation Effects 0.000 claims description 6
- 229910052684 Cerium Inorganic materials 0.000 claims description 3
- 229910052693 Europium Inorganic materials 0.000 claims description 3
- 229910004283 SiO 4 Inorganic materials 0.000 claims description 3
- 150000002500 ions Chemical class 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 229910015802 BaSr Inorganic materials 0.000 claims description 2
- 229910021645 metal ion Inorganic materials 0.000 claims description 2
- 229910052771 Terbium Inorganic materials 0.000 claims 1
- 229910000420 cerium oxide Inorganic materials 0.000 description 15
- BMMGVYCKOGBVEV-UHFFFAOYSA-N oxo(oxoceriooxy)cerium Chemical compound [Ce]=O.O=[Ce]=O BMMGVYCKOGBVEV-UHFFFAOYSA-N 0.000 description 15
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 10
- 239000000843 powder Substances 0.000 description 9
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 6
- 150000001875 compounds Chemical class 0.000 description 6
- 239000001301 oxygen Substances 0.000 description 6
- 229910052760 oxygen Inorganic materials 0.000 description 6
- 238000005245 sintering Methods 0.000 description 6
- 239000000203 mixture Substances 0.000 description 5
- 238000000862 absorption spectrum Methods 0.000 description 4
- 238000009877 rendering Methods 0.000 description 4
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 3
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 3
- ZMIGMASIKSOYAM-UHFFFAOYSA-N cerium Chemical compound [Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce][Ce] ZMIGMASIKSOYAM-UHFFFAOYSA-N 0.000 description 3
- 239000001257 hydrogen Substances 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- -1 metals Ions Chemical class 0.000 description 3
- 150000004767 nitrides Chemical class 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 229910052707 ruthenium Inorganic materials 0.000 description 3
- 150000003568 thioethers Chemical class 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 2
- 229910052788 barium Inorganic materials 0.000 description 2
- 229910052791 calcium Inorganic materials 0.000 description 2
- 239000007789 gas Substances 0.000 description 2
- 238000005286 illumination Methods 0.000 description 2
- XNGIFLGASWRNHJ-UHFFFAOYSA-L phthalate(2-) Chemical compound [O-]C(=O)C1=CC=CC=C1C([O-])=O XNGIFLGASWRNHJ-UHFFFAOYSA-L 0.000 description 2
- MZLGASXMSKOWSE-UHFFFAOYSA-N tantalum nitride Chemical compound [Ta]#N MZLGASXMSKOWSE-UHFFFAOYSA-N 0.000 description 2
- 101150027751 Casr gene Proteins 0.000 description 1
- KRKNYBCHXYNGOX-UHFFFAOYSA-K Citrate Chemical compound [O-]C(=O)CC(O)(CC([O-])=O)C([O-])=O KRKNYBCHXYNGOX-UHFFFAOYSA-K 0.000 description 1
- 229910052688 Gadolinium Inorganic materials 0.000 description 1
- 241000227425 Pieris rapae crucivora Species 0.000 description 1
- 229910004298 SiO 2 Inorganic materials 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- 238000004020 luminiscence type Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 229910017604 nitric acid Inorganic materials 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 125000005498 phthalate group Chemical class 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
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- C—CHEMISTRY; METALLURGY
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- C09K—MATERIALS FOR MISCELLANEOUS APPLICATIONS, NOT PROVIDED FOR ELSEWHERE
- C09K11/00—Luminescent, e.g. electroluminescent, chemiluminescent materials
- C09K11/08—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials
- C09K11/77—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals
- C09K11/7766—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing two or more rare earth metals
- C09K11/7775—Germanates
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L33/48—Semiconductor devices having potential barriers specially adapted for light emission; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by the semiconductor body packages
- H01L33/50—Wavelength conversion elements
- H01L33/501—Wavelength conversion elements characterised by the materials, e.g. binder
- H01L33/502—Wavelength conversion materials
- H01L33/504—Elements with two or more wavelength conversion materials
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02B—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO BUILDINGS, e.g. HOUSING, HOUSE APPLIANCES OR RELATED END-USER APPLICATIONS
- Y02B20/00—Energy efficient lighting technologies, e.g. halogen lamps or gas discharge lamps
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- Inorganic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Organic Chemistry (AREA)
- Luminescent Compositions (AREA)
Description
本發明係關於一種螢光材料,更特別關於此種材料於白光發光裝置之應用。
利用具省電、低污染與壽命長等優點之白光發光二極體(light emitting diodes;LEDs)作為照明光源巳是現代照明主要發展趨勢。為取得理想的照明光源,除LED本身亮度外,所選用之螢光體亦為影響光源整體發光效率之關鍵因素。
目前市面上常見白光LED為藍色LED(發射波長為460-480nm)配合黃色螢光粉,因缺乏紅色成份,其演色性較差。故搭配紅色、黃色螢光粉及組合之白光LED將比只含有單一黃色螢光粉之白光LED具更高演色性。但目前市面常見的藍光激發之紅色螢光粉以氮化物及硫化物為主(發射波長為620-650nm),氮化物最大優點是穩定度高,但其原料為氮化鍶及氮化鋇,再加上有些氮化物螢光粉甚至需要高溫高壓製程,所以成本極為高昂。硫化物雖然成本較低,但其具極差之化學穩定性,故不適合做為LED之螢光粉。近來利用矽酸鹽材料之橘紅色螢光粉搭配黃色螢光粉及藍色LED而成之高演色性白光LED,則是不錯的選擇。目前市面上常見矽酸鹽橘紅光螢光粉為BOS系列之BOS600(CaSr)2
SiO4
:Eu2+
螢光粉(發射波長為580-600nm),其成本較低發光效率也不差,化學穩定性也優於硫化物,但缺點是熱穩定性仍不夠好。綜上所述,目前亟需發光效率不差、成本低、及熱穩定性佳的橘紅色螢光粉。
本發明一實施例提供一種螢光材料,具有化學式如下:(Sr1-a-b-c
Ma
Tmb
Euc
)3
Si1-d
Ged
O5
;其中Sr、M、Tm、及Eu為二價金屬離子,且M係Ca、Ba、Mg、或上述之組合;Si及Ge為四價離子;0a0.5;0b0.03;0<c0.1;以及0<d0.005。
本發明一實施例提供一種白光發光裝置,包括藍光激發光源;以及黃色螢光材料與上述之螢光材料。
本發明揭露一系列矽酸鹽螢光材料,其化學式如式1:
(Sr1-a-b-c
Ma
Tmb
Euc
)3
Si1-d
Ged
O5
(式1)
在式1中,Sr、M、Tm、及Eu為二價金屬離子,且M為Ca、Ba、Mg、或上述之組合。Si與Gd為四價離子。0a0.5;0b0.03;0<c0.1;以及0<d0.005。上述螢光材料之主要機制為在原來橘黃光螢光材料之主體Sr3
SiO5
中,另外摻雜元素來增加其發光效率。
若式1中的螢光材料化學式中的a=b=0時,上述之螢光材料的化學式為(Sr1-c
Euc
)3
Si1-d
Ged
O5
,其發射光譜為580nm±5nm。
若式1中的螢光材料化學式中的a=0,且0<b0.03時,上述之螢光材料的化學式為(Sr1-b-c
Tmb
Euc
)3
Si1-d
Ged
O5
,其發射光譜為580nm±5nm。
若式1中的螢光材料化學式中的M為Ba,0.1a0.5,且0<b0.03及0<d0.005時,上述之螢光材料的化學式為(Sr1-a-b-c
Baa
Tmb
Euc
)3
Si1-d
Ged
O5
,其發射光譜為600nm±5nm。
上述螢光材料可與黃色螢光材料如Y3
Al5
O12
:Ce(簡稱YAG)、Tb3
Al5
O12
:Ce、(BaSr)2
SiO4
:Eu、或上述之組合結合,搭配藍光的激發光源如發光二極體或雷射二極體,即完成白光發光裝置。在本發明一實施例中,此白光發光裝置為暖色系的白光發光裝置。
此外,本發明亦提供上述矽酸鹽螢光材料之製造方法,包含以下步驟:首先,混合以下成份得到混合物:(1)具有鍶的含氧化合物;(2)具有矽的含氧化合物;(3)具有鍺的含氧化合物;(4)具有銪的含氧化合物;與(5)具有銩及/或M的含氧化合物。接著對混合物進行燒結,且燒結溫度介於1300℃-1600℃之間。當混合物升溫至燒結溫度後,維持在燒結溫度下1至4小時,以燒結混合物。根據本發明之實施例,含氧化合物可為氧化物、碳酸化合物、或硝酸化合物。
為了讓本發明之上述和其他目的、特徵、和優點能更明顯易懂,下文特舉數實施例配合所附圖式,作詳細說明如下:
【實施例】
實施例1
依化學劑量比例取氧化鍶、氧化銪、氧化矽、及氧化鍺,均勻混合後研磨10分鐘,並放入坩鍋,置入高溫爐,於5%之氫氣與95%氮氣的混合氣體下加熱至1300℃~1600℃燒結,以製備不同Si/Ge比例的(Sr0.99
Eu0.01
)3
Si1-d
Ged
O5
,其中d分別為0、0.001、0.01、及0.05。第1a圖係不同Si/Ge比例的螢光材料(Sr0.99
Eu0.01
)3
Si1-d
Ged
O5
之吸收光譜,而第1b圖係不同Si/Ge比例的螢光材料(Sr0.99
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜。當d為0時,(Sr0.09
Eu0.01
)3
SiO5
之激發波段介於深紫外光的250nm至綠光的550nm左右,發射光譜則為橘黃的580nm左右。當Ge之摻雜量d=0.001時,其激發波段和發光波長並無改變,但可增加發光效率。適量添加Ge可增加長波段之激發效率,如第1a圖所示。
實施例2
依化學劑量比例取氧化鍶、氧化銪、氧化矽、氧化鍺、及氧化銩,均勻混合後研磨10分鐘,並放入坩鍋,置入高溫爐,於5%之氫氣與95%氮氣的混合氣體下加熱至1300℃~1600℃燒結,以製備不同Sr/Tm及Si/Ge比例的(Sr0.99-b
Tmb
Eu0.01
)3
Si1-d
Ged
O5
,其中(b,d)分別為(0,0)、(0.003,0)、(0,0.01)、及(0.003,0.001)。第2a圖係不同Sr/Tm及Si/Ge比例的螢光材料(Sr0.99-b
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之吸收光譜,而第2b圖係不同Sr/Tm及Si/Ge比例的螢光材料(Sr0
.99-b
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜。由第2b圖可知,不論添加Ge或Tm均能增加發光效率,但同時適量添加二種元素則可進一步增加螢光材料之發光效率。
實施例3
依化學劑量比例取氧化鍶、氧化銪、氧化矽、氧化鍺、氧化銩及氧化鋇,均勻混合後研磨10分鐘,並放入坩鍋,置入高溫爐,於5%之氫氣與95%氮氣的混合氣體下加熱至1300℃~1600℃燒結,以製備不同Sr/Ba/Tm及Si/Ge比例的(Sr0.99-a-b
Baa
Tmb
Eu0.01
)3
Si1-d
Ged
O5
,其中(a,b,d)分別為(0,0,0)、(0,0.003,0.001)、(0.1,0.003,0.001)、(0.17,0.003,0.001)、及(0.23,0.003,0.001)。第3圖係不同Sr/Ba/Tm及Si/Ge比例的螢光材料(Sr0.99-a-b
Baa
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜。
因藍光激發黃光螢光粉之白光LED需要橘紅色螢光粉來增加其演色性,進一步添加鹼土金屬元素Ba的添加來位移發光波長,如圖3所示。摻雜Tm及Ge可增加發光效率,而摻雜Ba可位移發光。無掺雜之螢光材料發射580nm左右的橘黃光,而添加Ba之螢光材料的放射光譜將位移至597nm之橘紅光。第4圖則為上述產物的X光繞射圖。由圖中得知除了少許不發光原料之SiO2
的相,絶大部分是由Sr3
SiO5
所組成。另上述之橘紅色的螢光材料搭配黃色的螢光材料YAG及藍光LED時,可形成色溫3000K之暖白光LED,如第5圖所示。
雖然本發明已以數個較佳實施例揭露如上,然其並非用以限定本發明,任何熟習此技藝者,在不脫離本發明之精神和範圍內,當可作任意之更動與潤飾,因此本發明之保護範圍當視後附之申請專利範圍所界定者為準。
第1a圖係本發明一實施例中,不同Si/Ge比例的螢光材料(Sr0.99
Eu0.01
)3
Si1-d
Ged
O5
之吸收光譜;
第1b圖係本發明一實施例中,不同Si/Ge比例的螢光材料(Sr0.99
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜;
第2a圖係本發明一實施例中,不同Sr/Tm及Si/Ge比例的螢光材料(Sr0.99-b
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之吸收光譜;
第2b圖係本發明一實施例中,不同Sr/Tm及Si/Ge比例的螢光材料(Sr0.99-b
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜;
第3圖係本發明一實施例中,不同Sr/Ba/Tm及Si/Ge比例的螢光材料(Sr0.99-a-b
Baa
Tmb
Eu0.01
)3
Si1-d
Ged
O5
之發射光譜;
第4圖係本發明一實施例中,(Sr0.86
Ba0.1
Tm0.003
Eu0.01
)3
Si0.999
Ge0.001
O5
之之X-ray繞射圖;以及
第5圖係本發明一實施例中,黃色螢光材料YAG、(Sr0.757
Ba0.23
Tm0.003
Eu0.01
)3
Si0.999
Ge0.001
O5
、藍光LED、及上述三者組合成的白光發光裝置的CIE座標。
Claims (5)
- 一種螢光材料,具有化學式如下:(Sr1-a-b-c Ma Tmb Euc )3 Si1-d Ged O5 ;其中Sr、M、Tm、及Eu為二價金屬離子,且M係Ca、Ba、Mg、或上述之組合;Si及Ge為四價離子;0a0.5;0<b0.03;0<c0.1;以及0<d0.005。
- 如申請專利範圍第1項所述之螢光材料,具有化學式如下:(Sr1-b-c Tmb Euc )3 Si1-d Ged O5 ,其發射光譜為580nm±5nm;其中0<b0.03。
- 如申請專利範圍第1項所述之螢光材料,具有化學式如下:(Sr1-a-b-c Baa Tmb Euc )3 Si1-d Ged O5 ,其發射光譜為600nm±5nm;其中0.1≦a≦0.5;0<b≦0.03。
- 一種白光發光裝置,包括:一藍光激發光源;以及一黃色螢光材料與申請專利範圍第1項所述之螢光材料。
- 如申請專利範圍第4項所述之白光發光裝置,其中該黃色螢光材料為Y3 Al5 O12 :Ce、Tb3 Al5 O12 :Ce、(BaSr)2 SiO4 :Eu、或上述之組合。
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TW100132035A TWI421328B (zh) | 2011-09-06 | 2011-09-06 | 螢光材料與白光發光裝置 |
CN201110307076.5A CN102977884B (zh) | 2011-09-06 | 2011-10-08 | 荧光材料与白光发光装置 |
US13/288,773 US8721924B2 (en) | 2011-09-06 | 2011-11-03 | White light emitting devices utilizing phosphors |
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