CA2575841A1 - Novel silicate-based yellow-green phosphors - Google Patents
Novel silicate-based yellow-green phosphors Download PDFInfo
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- CA2575841A1 CA2575841A1 CA002575841A CA2575841A CA2575841A1 CA 2575841 A1 CA2575841 A1 CA 2575841A1 CA 002575841 A CA002575841 A CA 002575841A CA 2575841 A CA2575841 A CA 2575841A CA 2575841 A1 CA2575841 A1 CA 2575841A1
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- 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
- C09K11/0883—Arsenides; Nitrides; Phosphides
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- A—HUMAN NECESSITIES
- A44—HABERDASHERY; JEWELLERY
- A44B—BUTTONS, PINS, BUCKLES, SLIDE FASTENERS, OR THE LIKE
- A44B19/00—Slide fasteners
- A44B19/02—Slide fasteners with a series of separate interlocking members secured to each stringer tape
- A44B19/04—Stringers arranged edge-to-edge when fastened, e.g. abutting stringers
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- 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
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/7734—Aluminates
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- C—CHEMISTRY; METALLURGY
- C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
- 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
- C09K11/7728—Luminescent, e.g. electroluminescent, chemiluminescent materials containing inorganic luminescent materials containing rare earth metals containing europium
- C09K11/77342—Silicates
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- A—HUMAN NECESSITIES
- A44—HABERDASHERY; JEWELLERY
- A44D—INDEXING SCHEME RELATING TO BUTTONS, PINS, BUCKLES OR SLIDE FASTENERS, AND TO JEWELLERY, BRACELETS OR OTHER PERSONAL ADORNMENTS
- A44D2203/00—Fastening by use of magnets
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L33/00—Semiconductor devices with at least one potential-jump barrier or surface barrier 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 with at least one potential-jump barrier or surface barrier 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
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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
Abstract
Novel phosphor systems are disclosed having the formula A2SiO4:Eu2+D, where A
is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, P, S and N. In one embodiment, the novel phosphor has the formula (Sr1-x-yBaxMy)2 SiO4: Eu2+F (where M is one of Ca, Mg, Zn, or Cd in an amount ranging from 0<y<0.5). The phosphor is configured to absorb visible light from a blue LED, and luminescent light from the phosphor plus light from the blue LED may be combined to form white light. The novel phosphors can emit light at intensities greater than either conventionally known YAG compounds, or silicate-based phosphors that do not contain the inventive dopant ion.
is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, P, S and N. In one embodiment, the novel phosphor has the formula (Sr1-x-yBaxMy)2 SiO4: Eu2+F (where M is one of Ca, Mg, Zn, or Cd in an amount ranging from 0<y<0.5). The phosphor is configured to absorb visible light from a blue LED, and luminescent light from the phosphor plus light from the blue LED may be combined to form white light. The novel phosphors can emit light at intensities greater than either conventionally known YAG compounds, or silicate-based phosphors that do not contain the inventive dopant ion.
Claims (24)
1. A silicate-based yellow-green phosphor having the formula A2SiO4:Eu2+D, wherein:
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, P, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent.
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, P, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent.
2. The silicate-based phosphor of claim 1, wherein the phosphor is configured to absorb radiation in a wavelength ranging from about 280 nm to 490 nm.
3. The silicate-based phosphor of claim 1, wherein the phosphor emits visible light having a wavelength ranging from about 460 nm to 590 nm.
4. The silicate-based phosphor of claim 1, wherein the phosphor has the formula (Sr1-x-y Ba x M y)2 SiO4: Eu2+D, where M is at least one of an element selected from the group consisting of Ca, Mg, Zn, and Cd, and where 0<=x<=1;
0<=y<=1 when M is Ca;
0<=y<=1 when M is Mg; and 0<=y<=1 when M is selected from the group consisting of Zn and Cd.
0<=y<=1 when M is Ca;
0<=y<=1 when M is Mg; and 0<=y<=1 when M is selected from the group consisting of Zn and Cd.
5. The silicate-based phosphor of claim 1, wherein D is F.
6. The silicate-based phosphor of claim 1, wherein the phosphor has the formula (Sr1-x-y Ba x M y)2 SiO4: Eu2+F, where M is at least one of an element selected from the group of Ca, Mg, Zn,Cd, and where 0<=x<=0.3;
0<=y<=0.5 when M is Ca;
0<=y<=0.1 when M is Mg; and 0<=y<=0.5 when M is selected from the group consisting of Zn and Cd.
0<=y<=0.5 when M is Ca;
0<=y<=0.1 when M is Mg; and 0<=y<=0.5 when M is selected from the group consisting of Zn and Cd.
7. The silicate-based phosphor of claim 6, wherein the phosphor emits light in the yellow region of the electromagnetic spectrum, and has a peak emission wavelength ranging from about 540 to 590 nm.
8. The silicate-based phosphor of claim 1, wherein the phosphor has the formula (Sr1-x-y Ba x M y)2 Si04: Eu2+F, where M is at least one of an element selected from the group consisting of Ca, Mg, Zn, and Cd, and where 0.3<=x<=1;
0<=y<=0.5 when M is Ca;
0<=y<=0.1 when M is Mg; and 0<=y<=0.5 when M is selected from the group consisting of Zn and Cd.
0<=y<=0.5 when M is Ca;
0<=y<=0.1 when M is Mg; and 0<=y<=0.5 when M is selected from the group consisting of Zn and Cd.
9. The silicate-based phosphor of claim 8, wherein the phosphor emits light in the green region of the electromagnetic spectrum, and has a peak emission wavelenth ranging from about 500 to 530 nm.
10. A white LED comprising:
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with a peak intensity in a wavelength ranging from about 530 to 590 nm.
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with a peak intensity in a wavelength ranging from about 530 to 590 nm.
11. A white LED comprising:
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 530 to 590 nm; and a green phosphor according to claim 9, the green phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 500 to 540 nm.
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 530 to 590 nm; and a green phosphor according to claim 9, the green phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 500 to 540 nm.
12. A white LED comprising:
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a green phosphor according to claim 9, the green phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 500 to 540 nm;
a red phosphor selected from the group consisting of CaS:Eu2+, SrS:Eu2+, MgO*MgF*GeO:Mn4+, and M x Si y N z:Eu+2, where M is selected from the group consisting of Ca, Sr, Ba, and Zn; Z=2/3x+4/3y, wherein the red phosphor is configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 590 to 690nm.
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a green phosphor according to claim 9, the green phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 500 to 540 nm;
a red phosphor selected from the group consisting of CaS:Eu2+, SrS:Eu2+, MgO*MgF*GeO:Mn4+, and M x Si y N z:Eu+2, where M is selected from the group consisting of Ca, Sr, Ba, and Zn; Z=2/3x+4/3y, wherein the red phosphor is configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 590 to 690nm.
13. A white LED comprising:
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with a peak intensity in a wavelength ranging from about 540 to 590 nm;
a red phosphor selected from the group consisting of CaS:Eu2+, SrS:Eu2+, MgO*MgF*GeO:Mn4+, and M x Si y N z:Eu+2, where M is selected from the group consisting of Ca, Sr, Ba, and Zn; and Z=2/3x+4/3y, wherein the red phosphor is configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 590 to 690nm.
a radiation source configured to emit radiation having a wavelength ranging from about 410 to 500 nm;
a yellow phosphor according to claim 7, the yellow phosphor configured to absorb at least a portion of the radiation from the radiation source and emit light with a peak intensity in a wavelength ranging from about 540 to 590 nm;
a red phosphor selected from the group consisting of CaS:Eu2+, SrS:Eu2+, MgO*MgF*GeO:Mn4+, and M x Si y N z:Eu+2, where M is selected from the group consisting of Ca, Sr, Ba, and Zn; and Z=2/3x+4/3y, wherein the red phosphor is configured to absorb at least a portion of the radiation from the radiation source and emit light with peak intensity in a wavelength ranging from about 590 to 690nm.
14. A composition comprising:
a silicate-based yellow phosphor having the formula A2SiO4:Eu2+D, wherein A is at least one divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd;
and D is an ion that is present in the yellow phosphor in an amount ranging from about 0.01 to 20 mole percent; and a blue phosphor;
wherein the yellow phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 540 nm to 590 nm; and the blue phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 480 to 510 nm.
a silicate-based yellow phosphor having the formula A2SiO4:Eu2+D, wherein A is at least one divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd;
and D is an ion that is present in the yellow phosphor in an amount ranging from about 0.01 to 20 mole percent; and a blue phosphor;
wherein the yellow phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 540 nm to 590 nm; and the blue phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 480 to 510 nm.
15. The composition of claim 10, wherein the blue phosphor is selected from the group consisting of silicate-based phosphors and aluminate-based phosphors.
16. The composition of claim 11, wherein the silicate-based blue phosphor has the formula Sr1-x-y Mg x Ba y SiO4:Eu2+F; and where 0.5<=x<=1.0; and 0<=y<=0.5.
17. The composition of claim 11, wherein the aluminate-based blue phosphor has the formula Sr1-x MgEu x Al10O17; and where 0.01<=x<=1Ø
18. A composition comprising:
a silicate-based green phosphor having the formula A2SiO4:Eu2+H, wherein A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and H is a negatively charged halogen ion that is present in the yellow phosphor in an amount ranging from about 0.01 to 20 mole percent;
a blue phosphor; and a red phosphor;
wherein the green phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 500nm to 540 nm; the blue phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 480 to 510 nm; and the red phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 775 to 620 nm.
a silicate-based green phosphor having the formula A2SiO4:Eu2+H, wherein A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and H is a negatively charged halogen ion that is present in the yellow phosphor in an amount ranging from about 0.01 to 20 mole percent;
a blue phosphor; and a red phosphor;
wherein the green phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 500nm to 540 nm; the blue phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 480 to 510 nm; and the red phosphor is configured to emit visible light with a peak intensity in a wavelength ranging from about 775 to 620 nm.
19. A method of preparing a silicate-based yellow phosphor having the formula A2SiO4:Eu2+D, wherein A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, P, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent, the method selected from the group consisting of a sol-gel method and a solid reaction method.
20. The method of claim 19, wherein the sol-gel method comprises:
a) dissolving a desired amount of an alkaline earth nitrate selected from the group consisting of Mg, Ca, Sr, and Ba-containing nitrates with a compound selected from the group consisting of Eu2O3 and BaF2 or other alkaline metal halides, in an acid, to prepare a first solution;
b) dissolving corresponding amount of a silica gel in de-ionized water to prepare a second solution;
c) stirring together the solutions produced in steps a) and b), and then adding ammonia to generate a gel from the mixture solution;
d) adjusting the pH of the solution produced in step c) to a value of about 9, and then stirring the solution continuously at about 60°C for about 3 hours;
e) drying the gelled solution of step d) by evaporation, and then decomposing the resulting dried gel at 500 to 700°C for about 60 minutes to decompose and acquire product oxides;
f) cooling and grinding the gelled solution of step e) with NH4F or other ammonia halides when alkaline earth metal halides are not used in step a) to produce a powder;
g) calcining/sintering the powder of step f) in a reduced atmosphere for about 6 to 10 hours, the sintering temperature ranging from about 1200 to 1400°C.
a) dissolving a desired amount of an alkaline earth nitrate selected from the group consisting of Mg, Ca, Sr, and Ba-containing nitrates with a compound selected from the group consisting of Eu2O3 and BaF2 or other alkaline metal halides, in an acid, to prepare a first solution;
b) dissolving corresponding amount of a silica gel in de-ionized water to prepare a second solution;
c) stirring together the solutions produced in steps a) and b), and then adding ammonia to generate a gel from the mixture solution;
d) adjusting the pH of the solution produced in step c) to a value of about 9, and then stirring the solution continuously at about 60°C for about 3 hours;
e) drying the gelled solution of step d) by evaporation, and then decomposing the resulting dried gel at 500 to 700°C for about 60 minutes to decompose and acquire product oxides;
f) cooling and grinding the gelled solution of step e) with NH4F or other ammonia halides when alkaline earth metal halides are not used in step a) to produce a powder;
g) calcining/sintering the powder of step f) in a reduced atmosphere for about 6 to 10 hours, the sintering temperature ranging from about 1200 to 1400°C.
21. The method of claim 19, wherein the solid reaction method comprises:
a) wet mixing desired amounts of alkaline earth oxides or carbonates (Mg, Ca, Sr, Ba), dopants of Eu2O3 and/or BaF2 or other alkaline earth metal halides, corresponding SiO2 and/or NH4F or other ammonia halides with a ball mill; and b) after drying and grinding, calcining and/or sintering the resulting powder was in a reduced atmosphere for about 6 to 10 hours, wherein the calcining/sintering temperature ranged from about 1200 to 1400°C.
a) wet mixing desired amounts of alkaline earth oxides or carbonates (Mg, Ca, Sr, Ba), dopants of Eu2O3 and/or BaF2 or other alkaline earth metal halides, corresponding SiO2 and/or NH4F or other ammonia halides with a ball mill; and b) after drying and grinding, calcining and/or sintering the resulting powder was in a reduced atmosphere for about 6 to 10 hours, wherein the calcining/sintering temperature ranged from about 1200 to 1400°C.
22. A silicate-based yellow-green phosphor having the formula A2SiO4 : Eu2+D, wherein:
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent.
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent.
23. A method of preparing a silicate-based yellow phosphor having the formula A2SiO4 : Eu2+D, wherein A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, S and N, wherein D is present in the phosphor in an amount ranging from about 0.01 to 20 mole percent, the method selected from the group consisting of a sol-gel method and a solid reaction method.
24. A silicate-based yellow-green phosphor having the formula (Al-x Eu x)2Si(O1-y D y)4, wherein:
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, S and N; and, 0.001<x<0.10; 0.01<y<0.2.
A is at least one of a divalent metal selected from the group consisting of Sr, Ca, Ba, Mg, Zn, and Cd; and D is a dopant selected from the group consisting of F, Cl, Br, I, S and N; and, 0.001<x<0.10; 0.01<y<0.2.
Applications Claiming Priority (5)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US10/912,741 | 2004-08-04 | ||
US10/912,741 US7267787B2 (en) | 2004-08-04 | 2004-08-04 | Phosphor systems for a white light emitting diode (LED) |
US10/948,764 | 2004-09-22 | ||
US10/948,764 US7311858B2 (en) | 2004-08-04 | 2004-09-22 | Silicate-based yellow-green phosphors |
PCT/US2004/039638 WO2006022792A2 (en) | 2004-08-04 | 2004-11-24 | Novel silicate-based yellow-green phosphors |
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CA2575841A1 true CA2575841A1 (en) | 2006-03-02 |
CA2575841C CA2575841C (en) | 2011-06-07 |
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CA2575841A Expired - Fee Related CA2575841C (en) | 2004-08-04 | 2004-11-24 | Novel silicate-based yellow-green phosphors |
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US (1) | US7311858B2 (en) |
EP (1) | EP1778816A4 (en) |
KR (4) | KR100538104B1 (en) |
AU (1) | AU2004322659B2 (en) |
BR (1) | BRPI0418982A (en) |
CA (1) | CA2575841C (en) |
MX (1) | MX2007001446A (en) |
TW (1) | TWI374926B (en) |
WO (1) | WO2006022792A2 (en) |
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KR100632144B1 (en) | 2006-10-11 |
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