Phosphors

• US 9,745,511 B2
• Filed: 07/09/2014
• Issued: 08/29/2017
• Est. Priority Date: 08/08/2013
• Status: Expired due to Fees

• Current Assignee: Merck Patent GmbH (Merck & Co., Inc.)
• Original Assignee: Merck Patent GmbH (Merck & Co., Inc.)
• Inventors: Winkler, Holger, Juestel, Thomas, Katelnikovas, Arturas, Dierkes, Tobias
• Primary Examiner(s): Anya, Igwe U
• Application Number:
  US14/909,760
• Publication Number:
  US 20160186056A1
• Time in Patent Office: 1,147 Days
• Field of Search: 257 98
• CPC Class Codes: C09K 11/77928 Silicon Aluminium Nitrides or Silicon Aluminium Oxynitrides
• CPC Class Codes: H01L 33/502 Wavelength conversion materials
• CPC Class Codes: H05B 33/14 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

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.

Claims

1. A compound of formula (1):

(EA)_1-yMSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

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-xAl_xN_7-xO_x;

y Eu²⁺ where 0.004≦

x≦

1.0 are excluded from the invention.

2. The compound according to claim 1, which is of formula (2),

(Mg_aCa_bSr_cBa_d)_1-y(Y_eLu_f)Si_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

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_aCa_b)_1-yYSi_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

formula (2a)

(Mg_aCa_b)_1-yLuSi_4-xAl_xN_7-O_x;

yEu²⁺ 

 

formula (2b)

(Mg_aSr_c)_1-yYSi_4-zAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2c)

(Mg_aSr_c)_1-yLuSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2d)

(Ca_bSr_c)_1-yYSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2e)

(Ca_bSr_c)_1-yLuSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2f)

(Ca_bBa_d)_1-yYSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2g)

(Ca_bBa_d)_1-yLuSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2h)

(Sr_cBa_d)_1-yYSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2i)

(Sr_cBa_d)_1-yLuSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2j)

Mg_1-y(Y_dLU_e)Si_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2k)

Ca_1-y(Y_eLu_f)Si_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2l)

Sr_1-y(Y_eLu_f)Si_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (2m)

Ba_1-y(Y_eLu_f)Si_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

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-yMSi_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

formula (3)

Ca_1-yMSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

formula (4)

Ba_1-yMSi_4-xAl_xN_7-xO_x;

yEu²⁺ 

 

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-yLuSi_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

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-yMSi_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

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-xAl_xN_7-xO_x;

y Eu²⁺ 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-yMSi_4-xAl_xN_7-xO_x:

yEu²⁺ 

 

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-xAl_xN_7-x;

y Eu²⁺ 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.