IP Library Granted Patent US 10,125,315
Granted Patent B2
US 10,125,315 · App. 15/569,943 · Granted Nov 13, 2018

Phosphors and phosphor-converted LEDs

Inventors: Aleksander Zych (Darmstadt, DE); Ralf Petry (Griesheim, DE); Mathias Rapphahn (Greifswald, DE); Ingo Koehler (Darmstadt, DE); Stefan Tews (Greifswald, DE)
Assignee: Merck Patent GmbH
C09K11/7792C09K11/7734H01L33/502
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Quick Facts
Patent No.
US 10,125,315
App. No.
15/569,943
Granted
Nov 13, 2018
Kind
B2
Abstract

The present invention relates to pyrosilicate phosphors, to a process for the preparation thereof and to the use thereof as conversion phosphors. The present invention also relates to an emission-converting material comprising the conversion phosphor according to the invention, and to the use thereof in light sources, in particular pc-LEDs (phosphor converted light emitting devices). The present invention furthermore relates to light sources, in particular pc-LEDs, and to lighting units which comprise a primary light source and the emission-converting material according to the invention.

Claims (134)

1. Compound of formula (1),

(Ba 2-a-b-c-d M a A b RE c D d )(Mg 1-e-f-g-j M′ e A′ f RE′ g C′ j )(Si 2-h-i B′ h C″ i )(O 7+m-k-l X k N l )   Formula (1)

where the following applies to the symbols and indices used:

M is selected from the group consisting of Ca, Sr, Zn or mixtures of these elements;

A is selected from the group consisting of Na, K, Rb or mixtures of these elements;

RE is selected from the group consisting of La, Y, Gd or mixtures of these elements;

D is selected from the group consisting of Eu 2+ , Mn 2+ , Yb 2+ , Sm 2+ or mixtures of these elements;

M′ is selected from the group consisting of Zr, Hf or mixtures of these elements;

A′ is selected from the group consisting of Li, Na or mixtures of these elements;

RE′ is selected from the group consisting of Sc, Lu or mixtures of these elements;

C′ is selected from the group consisting of B, Al, Ga, In or mixtures of these elements;

B′ is selected from the group consisting of Ge, Sn or mixtures of these elements;

C″ is selected from the group consisting of B, Al, Ga, In or mixtures of these elements;

X is selected from the group consisting of F, Cl or mixtures of these elements;

N is nitrogen;

0≤a≤1.0;

0≤b≤0.6;

0≤c≤0.6;

0≤d≤2.0;

0≤e≤0.3;

0≤f≤0.3;

0≤g≤0.3;

0≤j≤0.6;

0≤h≤1.0;

0≤i≤0.6;

0≤k≤2.1;

0≤l≤2.1; and

−2.0≤m≤2.0;

with the proviso that b≠0 and/or c≠0 and/or e≠0 and/or g≠0 and/or with the proviso that f≠0 and k≠0 at the same time and/or with the proviso that f≠0 and j and/or i≠0 at the same time.

2. Compound according to claim 1 wherein the following applies for the indices used:

0≤a≤0.6;

0≤b≤0.4;

0≤c≤0.4;

0≤d≤1.0;

0≤e≤0.2;

0≤f≤0.2;

0≤g≤0.2;

0≤j≤0.4;

0≤h≤0.6;

0≤i≤0.4;

0≤k≤1.4;

0≤l≤1.4; and

−1.0≤m≤1.0;

with the proviso that b≠0 and/or c≠0 and/or e≠0 and/or g≠0 and/or with the proviso that f≠0 and k≠0 at the same time and/or with the proviso that f≠0 and j and/or i≠0 at the same time.

3. Compound according to claim 1 wherein the following applies to the indices used:

0≤a≤0.4;

0≤b≤0.2;

0≤c≤0.2;

0.01≤d≤0.2;

0≤e≤0.1;

0≤f≤0.1;

0≤g≤0.1;

0≤j≤0.2;

0≤h≤0.4;

0≤i≤0.2;

0≤k≤0.7;

0≤l≤0.7;

−0.5≤m≤0.5;

with the proviso that b≠0 and/or c≠0 and/or e≠0 and/or g≠0 and/or with the proviso that f≠0 and k≠0 at the same time and/or with the proviso that f≠0 and j and/or i≠0 at the same time.

4. Compound according to claim 1 , characterised in that a maximum of three of the indices a, b, c, e, f, g, j, h, I, k and l is ≠0.

5. Compound according claim 1 , characterised in that a maximum of two of the indices a, b, c, e, f, g, j, h, I, k and l is ≠0.

6. Compound according to claim 1 , selected from the compounds of formula (2),

(Ba 2-a-b-c-d M a K b La c Eu d )(Mg 1-e-f-g-j Zr e Li f Sc g C′ j )(Si 2-h-i Ge h C″ i )(O 7+m-k-l X k N l )   Formula (2)

where the following applies for the symbols and indices used:

M is selected from the group consisting of Ca, Sr or mixtures of these elements;

C′ is selected from the group consisting of Al, Ga or mixtures of these elements;

C″ is selected from the group consisting of Al, Ga or mixtures of these elements;

X is selected from the group consisting of F, Cl or mixtures of these elements;

N is nitrogen;

0≤a≤0.4;

0≤b≤0.2;

0≤c≤0.2;

0.005≤d≤0.4, more preferably 0.01≤d≤0.2;

0≤e≤0.1;

0≤f≤0.1;

0≤g≤0.1;

0≤j≤0.2;

0≤h≤0.4;

0≤i≤0.2;

0≤k≤0.7;

0≤l≤0.7;

−0.5≤m≤0.5;

with the proviso that b≠0 and/or c≠0 and/or e≠0 and/or g≠0 and/or with the proviso that f≠0 and k≠0 at the same time and/or with the proviso that f≠0 and j and/or i≠0 at the same time.

7. Compound according claim 1 , selected from the compounds of formulae (3) to (13),

(Ba 2-b-d A b D d )Mg Si 2 (O 7-b X b )  Formula (3)

(Ba 2-b-d A b D a )(Mg 1-b RE′ b )Si 2 O 7   Formula (4)

(Ba 2-b-d A b D d )Mg Si 2 O 7-0.5b   Formula (5)

(Ba 2-c-d RE c D d )Mg Si 2 (O 7-c N c )  Formula (5)

(Ba 2-d D d )(Mg 1-g RE′ g )Si 2 (O 7-g N g )  Formula (7)

(Ba 2-d D d )(Mg 1-e M′ e )Si 2 O 7+e   Formula (8)

(Ba 2-d-0.5e D d )(Mg 1-e M′ e )Si 2 O 7+0.5e   Formula (9)

(Ba 2-d D d )(Mg 1-f A′ f )Si 2 (O 7-f X f )  Formula (10)

(Ba 2-d D d )(Mg 1-2f A′ f C′ f )Si 2 O 7   Formula (11)

(Ba 2-d D d )(Mg 1-f A′ f )(Si 2-f C″ f )O 7   Formula (12)

(Ba 2-d D d )(Mg 1-2e M′ e RE′ e )Si 2 (O 7-e N e )  Formula (13)

where the symbols and indices have the meanings given in claim 1 and furthermore:

b≠0 in formula (3), (4) and (5),

c≠0 in formula (6),

g≠0 in formula (7),

e≠0 in formula (8) and (9),

f≠0 in formula (10), (11) and (12), and

e≠0 in formula (13).

8. Compound according claim 1 , selected from the compounds of formulae (3a) to (13a),

(Ba 2-b-d K b Eu d )Mg Si 2 (O 7-b F b )  Formula (3a)

(Ba 2-b-d K b Eu d )Mg Si 2 (O 7-b Cl b )  Formula (3b)

(Ba 2-b-d K b Eu d )(Mg 1-b Sc b )Si 2 O 7   Formula (4a)

(Ba 2-b-d K b Eu d )Mg Si 2 O 7-0.5b   Formula (5a)

(Ba 2-c-d La c Eu d )Mg Si 2 (O 7-c N c )  Formula (6a)

(Ba 2-d Eu d )(Mg 1-g Sc g )Si 2 (O 7-g N g )  Formula (7a)

(Ba 2-d Eu d )(Mg 1-e Zr e )Si 2 O 7+e   Formula (8a)

(Ba 2-d-0.5e Eu d )(Mg 1-e Zr′ e )Si 2 O 7+0.5e   Formula (9a)

(Ba 2-d Eu d )(Mg 1-f Li f )Si 2 (O 7-f F f )  Formula (10a)

(Ba 2-d Eu d )(Mg 1-f Li f )Si 2 (O 7-f Cl f )  Formula (10b)

(Ba 2-d Eu d )(Mg 1-2f Li f Al f )Si 2 O 7   Formula (11a)

(Ba 2-d Eu d )(Mg 1-2f Li f Ga f )Si 2 O 7   Formula (11b)

(Ba 2-d Eu d )(Mg 1-f Li f )(Si 2-f Al f )O 7   Formula (12a)

(Ba 2-d Eu d )(Mg 1-f Li f )(Si 2-f Ga f )O 7   Formula (12b)

(Ba 2-d Eu d )(Mg 1-2e Zr e Sc e )Si 2 (O 7-e N e )  Formula (13a)

where the symbols and indices have the meanings given in claim 1 and furthermore:

b≠0 in formula (3a), (3b), (4a) and (5a),

c≠0 in formula (6a),

g≠0 in formula (7a),

e≠0 in formula (8a) and (9a),

f≠0 in formula (10a), (10b), (11a), (11b), (12a) and (12b), and

e≠0 in formula (13a).

9. Compound according claim 1 , characterised in that the compound is coated.

10. Process for the preparation of a compound according to claim 1 , comprising the steps:

a) preparation of a mixture comprising all elements, which should be incorporated into the compound; and

b) calcination of the mixture at elevated temperature.

11. Process according to claim 10 , characterised in that a fluxing agent is used, which is selected from the group of ammonium halides, alkaline-earth metal fluorides, carbonates, alkoxides, oxalates and/or boric acid.

12. A conversion phosphor, in particular for the partial or complete conversion of the violet or near-UV emission of a light-emitting diode into light having a longer wavelength, which comprises a compound of claim 1 .

13. Light source which comprises at least one primary light source and at least one compound according to claim 1 .

14. Light source according to claim 13 , wherein the primary light source is a luminescent indium aluminium gallium nitride or a luminescent arrangement based on ZnO, TCO (transparent conducting oxide) or SiC, or a near-UV or violet laser, or a source which exhibits electroluminescence and/or photoluminescence, or a plasma or discharge source.

15. Lighting unit, in particular for the backlighting of display devices, characterised in that it comprises at least one light source according to claim 13 .

Assignments (2)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 3, 2020
From: MERCK PATENT GMBH
To: LITEC-VERMÖGENSVERWALTUNGSGESELLSCHAFT MBH
Reel/Frame 054256/0363 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 29, 2017
From: ZYCH, ALEKSANDER; PETRY, RALF; RAPPHAHN, MATHIAS; KOEHLER, INGO; TEWS, STEFAN
To: MERCK PATENT GMBH
Reel/Frame 044251/0717 →
Priority Claims (1)
EP 15001236 · Apr 27, 2015 · regional
Continuity (1)
Related Publication 20180155621A1 · Jun 7, 2018