Composite ceramic which comprises a conversion phosphor and a material having a negative coefficient of thermal expansion
The present invention relates to a composite ceramic which comprises a conversion phosphor and a further material, characterized in that the further material has a negative coefficient of thermal expansion, and to a process for the preparation thereof. Furthermore, the present invention also relates to the use of the composite ceramic according to the invention as emission-converting material, preferably in a white light source, and to a light source, a lighting unit and a display device.
1. Composite ceramic which comprises a conversion phosphor and a further material, wherein the further material has a negative coefficient of thermal expansion which is in the range from 1*10 −6 to 12*10 −6 K −1 in the case of a temperature change in the range from 20° C. to 200° C.
2. Composite ceramic according to claim 1 , in which the conversion phosphor is a Ce-, Eu- and/or Mn-containing material.
3. Composite ceramic according to claim 1 , in which the conversion phosphor is a Ce-containing material.
4. Composite ceramic according to claim 3 , in which the Ce-containing material is a Ce-containing garnet which has the formula E 3 G 2 (TO 4 ) 3 :Ce, where E is selected from the group consisting of Y, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Lu and mixtures thereof, and G and T are each selected, independently of one another, from the group consisting of Al, Sc, Ga and mixtures thereof, or G and T together stand for the combination Mg/Si or the combination Mg/Ge, where Mg and Si or Mg and Ge respectively are present in the same molar proportions.
5. Composite material according to claim 1 , in which the further material is a tungstate or molybdate.
6. Composite ceramic according to claim 1 , in which the molar ratio of the conversion phosphor to the further material is in the range from 1:0.5 to 10:1.
7. Process for the preparation of a composite ceramic according to claim 1 , which comprises:
a) providing a conversion phosphor;
b) providing a material having a negative coefficient of thermal expansion;
c) mixing of the two components provided in steps a) and b) to give a mixture; and
d) sintering of the mixture.
8. Process according to claim 7 wherein the sintering is carried out at a temperature in the range from ⅔ to ⅚ of the melting temperature of the material having a negative coefficient of thermal expansion.
9. Process for the preparation of a composite ceramic according to claim 1 , which comprises:
a′) coating of a conversion phosphor with an oxide of aluminium;
b′) mixing of the coated conversion phosphor obtained in step a′) with a W- or Mo-containing component to give a mixture; and
c′) sintering of the mixture obtained in step b′) at a temperature in the range from 1000 to 1600° C., to obtain a composite ceramic which comprises a conversion phosphor and an aluminium tungstate or aluminium molybdate material which has a negative coefficient of thermal expansion in the range from 1*10 −6 to 12*10 −6 K −1 in the case of a temperature change in the range from 20° C. to 200° C.
10. An emission-converting material comprising a composite ceramic according to claim 1 .
11. A light source comprising an emission-converting material according to claim 10 .
12. Light source which comprises a composite ceramic according to claim 1 and a primary light source.
13. Lighting unit which comprises at least one light source according to claim 12 .
14. Composite ceramic according to claim 1 , in which the conversion phosphor is a Ce-, Eu- and/or containing material, which comprises 0.1 to 5 atom-% of Ce, Eu and/or Mn, based on the total number of atoms at the lattice sites which are replaced by the Ce, Eu and/or Mn in the Ce-, Eu- and/or Mn-containing material.
15. Composite ceramic according to claim 1 , in which the conversion phosphor is a Ce-containing garnet.
16. Composite material according to claim 1 , in which the further material is a tungstate or molybdate, which is selected from the group consisting of Al 2 W 3 O 12 , Y 2 W 3 O 12 , YAlW 3 O 12 , ZrW 2 O 8 , Al 2 Mo 3 O 12 , Y 2 Mo 3 O 12 , YAlMo 3 O 12 , ZrMo 2 O 8 , Al 2 WMo 2 O 12 , Y 2 WMo 2 O 12 , YAlWMo 2 O 12 , ZrWMoO 8 , Al 2 MoW 2 O 12 , Y 2 MoW 2 O 12 , YAlMoW 2 O 12 and mixtures thereof.
17. Composite ceramic according to claim 1 , in which the molar ratio of the conversion phosphor to the further material is in the range from 1:1 to 5:1.
18. Composite ceramic which comprises a conversion phosphor and a further material, wherein the further material is a tungstate or molybdate and has a negative coefficient of thermal expansion.
19. Composite material according to claim 18 , in which the further material is a tungstate or molybdate, which is selected from the group consisting of Al 2 W 3 O 12 , Y 2 W 3 O 12 , YAlW 3 O 12 , ZrW 2 O 8 , Al 2 Mo 3 O 12 , Y 2 Mo 3 O 12 , YAlMo 3 O 12 , ZrMo 2 O 8 , Al 2 WMo 2 O 12 , Y 2 WMo 2 O 12 , YAlWMo 2 O 12 , ZrWMoO 8 , Al 2 MoW 2 O 12 , Y 2 MoW 2 O 12 , YAlMoW 2 O 12 and mixtures thereof.