Phosphors

Patent metadata

Field	Value
Publication number	US-9745511-B2
Application number	US-201414909760-A
Country	US
Kind code	B2
Filing date	Jul 9, 2014
Priority date	Aug 8, 2013
Publication date	Aug 29, 2017
Grant date	Aug 29, 2017

Abstract

The present invention relates to europium-doped phosphors, to a process for the preparation thereof, and to the use of these compounds as conversion phosphors. The present invention furthermore relates to light-emitting devices which comprise the phosphor according to the invention.

First claim

The invention claimed is:

1. A compound of formula (1):
(EA) 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (1)

wherein
EA is Mg, Ca, Sr, or Ba or a mixture of two or more of the elements Mg, Ca, Sr and Ba;
M is Y, or Lu or a mixture of Y and Lu;
0.004≦x≦3.0;
0<y≦0.25;
with the proviso that compounds of formula SrYSi 4-x Al x N 7-x O x :y Eu 2+ where 0.004≦x≦1.0 are excluded from the invention.

2. The compound according to claim 1 , which is of formula (2),
(Mg a Ca b Sr c Ba d ) 1-y (Y e Lu f )Si 4-x Al x N 7-x O x :y Eu 2+   formula (2)

where x and y have the meanings given for the compound of formula (1) and furthermore:
0≦a≦1;
0≦b≦1;
0≦c≦1;
0≦d≦1;
a+b+c+d=1;
0≦e≦1;
0≦f≦1;
e+f=1; and
at least three of a, b, c, d, e and f are >0.

3. The compound according to claim 1 , which is one of formulae (2a) to (2n),
(Mg a Ca b ) 1-y YSi 4-x Al x N 7-x O x :y Eu 2+   formula (2a)

(Mg a Ca b ) 1-y LuSi 4-x Al x N 7- O x :y Eu 2+   formula (2b)

(Mg a Sr c ) 1-y YSi 4-z Al x N 7-x O x :y Eu 2+   formula (2c)

(Mg a Sr c ) 1-y LuSi 4-x Al x N 7-x O x :y Eu 2+   formula (2d)

(Ca b Sr c ) 1-y YSi 4-x Al x N 7-x O x :y Eu 2+   formula (2e)

(Ca b Sr c ) 1-y LuSi 4-x Al x N 7-x O x :y Eu 2+   formula (2f)

(Ca b Ba d ) 1-y YSi 4-x Al x N 7-x O x :y Eu 2+   formula (2g)

(Ca b Ba d ) 1-y LuSi 4-x Al x N 7-x O x :y Eu 2+   formula (2h)

(Sr c Ba d ) 1-y YSi 4-x Al x N 7-x O x :y Eu 2+   formula (2i)

(Sr c Ba d ) 1-y LuSi 4-x Al x N 7-x O x :y Eu 2+   formula (2j)

Mg 1-y (Y d LU e )Si 4-x Al x N 7-x O x :y Eu 2+   formula (2k)

Ca 1-y (Y e Lu f )Si 4-x Al x N 7-x O x :y Eu 2+   formula (2l)

Sr 1-y (Y e Lu f )Si 4-x Al x N 7-x O x :y Eu 2+   formula (2m)

Ba 1-y (Y e Lu f )Si 4-x Al x N 7-x O x :y Eu 2+   formula (2n)

where x and y have the meanings given for the compound of formula (1) and furthermore:
0<a≦1;
0<b≦1;
0<c≦1;
0<d≦1;
0<e≦1;
0<f≦1;
a+b=1 in formulae (2a) and (2b);
a+c=1 in formulae (2c) and (2d);
b+c=1 in formulae (2e) and (2f);
b+d=1 in formulae (2g) and (2h);
c+d=1 in formulae (2i) and (2j); and
e+f=1 in formulae (2k) to (2n).

4. The compound according to claim 3 , wherein the Mg:Ca, Mg:Sr, Ca:Sr, Ca:Ba or Sr:Ba ratio, based on the molar amounts, in formulae (2a) to (2j) is between 50:1 and 1:50, and the Y:Lu ratio, based on the molar amounts, in the formulae (2k) to (2n) is between 50:1 and 1:50.

5. The compound according to claim 3 , wherein the Mg:Ca, Mg:Sr, Ca:Sr, Ca:Ba or Sr:Ba ratio, based on the molar amounts, in formulae (2a) to (2j) is between 10:1 and 1:10, and the Y:Lu ratio, based on the molar amounts, in the formulae (2k) to (2n) is between 5:1 and 1:5.

6. The compound according to claim 1 , which is one of formula (3), (4) or (5),
Mg 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (3)

Ca 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (4)

Ba 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (5)

where M, x and y have the meanings given for the compound of formula (1).

7. The compound according to claim 1 , which is of formula (6),
(EA) 1-y LuSi 4-x Al x N 7-x O x :y Eu 2+   formula (6)

where EA, x and y have the meanings given for the compound of formula (1).

8. The compound according to claim 1 , wherein 0.5≦x≦2.0.

9. The compound according claim 1 , wherein 0<y≦0.20.

10. A process for preparing the compound according to claim 1 , comprising:
a) preparing a mixture of an Mg, Ca, Sr and/or Ba compound, a Y and/or Lu compound, an Si compound, an Al compound and an Eu compound, where at least one of these compounds is in the form of a nitride and at least one of these compounds is in the form of an oxide; and
b) calcining the mixture under non-oxidizing conditions.

11. The compound according to claim 1 , which has a coating on its the surface.

12. An emission-converting material comprising at least one compound according to claim 1 and optionally one or more further conversion phosphors.

13. A method for converting light in a light source, comprising achieving said conversion by a conversion phosphor comprising a compound according to claim 1 .

14. The compound according to claim 1 , wherein 1.3≦x≦1.7.

15. The compound according claim 1 , wherein 0.02≦y≦0.16.

16. The compound according to claim 1 , which has a metal oxide or a nitride coating on its surface.

17. An emission-converting material comprising at least one compound according to claim 1 and one or more further conversion phosphors.

18. A shaped body or ceramic comprising a compound of formula (1) or an emission-converting material comprising said compound and optionally comprising one or more further conversion phosphors
(EA) 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (1)

wherein
EA is Mg, Ca, Sr, or Ba or a mixture of two or more of the elements Mg, Ca, Sr and Ba;
M is Y, or Lu or a mixture of Y and Lu;
0.004≦x≦3.0;
0<y≦0.25;
with the proviso that compounds of formula SrYSi 4-x Al x N 7-x O x :y Eu 2+ where 0.004≦x≦1.0 are excluded from the invention.

19. A light source, comprising a primary light source and a at least one compound of formula (1) or an emission-converting material or a shaped body or ceramic comprising said compound and optionally comprising one or more further conversion phosphors
(EA) 1-y MSi 4-x Al x N 7-x O x :y Eu 2+   formula (1)

wherein
EA is Mg, Ca, Sr, or Ba or a mixture of two or more of the elements Mg, Ca, Sr and Ba;
M is Y, or Lu or a mixture of Y and Lu;
0.004≦x≦3.0;
0<y≦0.25;
with the proviso that compounds of formula SrYSi 4-x Al x N 7-x :y Eu 2+ where 0.004≦x≦1.0 are excluded from the invention.

20. A lighting unit comprising at least one light source according to claim 19 .

Assignees

• Merck Patent Gmbh

Inventors

• Winkler Holger
• Juestel Thomas
• Katelnikovas Arturas
• Dierkes Tobias

Classifications

• H05B33/14 Primary

  characterised by the chemical or physical composition or the arrangement of the electroluminescent material {, or by the simultaneous addition of the electroluminescent material in or onto the light source} · CPC title

• C09K11/77928 Primary

  Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides · CPC title

• H01L33/502

  Electricity · mapped topic

• C09K11/7792 Primary

  Aluminates · CPC title

• H10H20/8512

  Wavelength conversion materials · CPC title