Method for producing nitride fluorescent material, nitride fluorescent material and light emitting device
Disclosed are a production method for a nitride fluorescent material, a nitride fluorescent material and a light emitting device. The production method is for producing a nitride fluorescent material that has, as a fluorescent material core, a calcined body having a composition containing at least one element M a selected from the group consisting of Sr, Ca, Ba and Mg, at least one element M b selected from the group consisting of Li, Na and K, at least one element M c selected from the group consisting of Eu, Ce, Tb and Mn, and Al, and optionally Si, and N, and the method includes preparing a calcined body having the above-mentioned composition, bringing the calcined body into contact with a fluorine-containing substance, and subjecting it to a first heat treatment at a temperature of 100° C. or higher and 500° C. or lower to form a fluoride-containing first film on the calcined body, and forming on the calcined body, a second film that contains a metal oxide containing at least one metal element M2 selected from the group consisting of Si, Al, Ti, Zr, Sn and Zn and subjecting it to a second heat treatment at a temperature in a range of higher than 250° C. and 500° C. or lower.
1. A method for producing a nitride fluorescent material, that comprises, as a fluorescent material core, a calcined body having a composition comprising at least one element M a selected from the group consisting of Sr, Ca, Ba and Mg, at least one element M b selected from the group consisting of Li, Na and K, at least one element M c selected from the group consisting of Eu, Ce, Tb and Mn, and Al, and optionally Si, and N;
the method comprising:
preparing a calcined body having said composition comprising at least one element M a selected from the group consisting of Sr, Ca, Ba and Mg, at least one element M b selected from the group consisting of Li, Na and K, at least one element M c selected from the group consisting of Eu, Ce, Tb and Mn, and Al, and optionally Si, and N,
bringing the calcined body into contact with a fluorine-containing substance, and subjecting the calcined body to a first heat treatment at a temperature in a range of 100° C. or higher and 500° C. or lower to form a fluoride-containing first film on the calcined body, and
forming on the calcined body, a second film that comprises a metal oxide comprising at least one metal element M2 selected from the group consisting of Si, Al, Ti, Zr, Sn and Zn and subjecting the calcined body to a second heat treatment at a temperature in a range of higher than 250° C. and 500° C. or lower.
2. The method for producing a nitride fluorescent material according to claim 1 , wherein the fluorine-containing substance is at least one selected from the group consisting of F 2 , CHF 3 , CF 4 , NH 4 HF 2 , NH 4 F, SiF 4 , KrF 2 , XeF 2 , XeF 4 and NF 3 .
3. The method for producing a nitride fluorescent material according to claim 1 , wherein the second heat treatment is carried out in air or in an inert gas atmosphere.
4. The method for producing a nitride fluorescent material according to claim 1 , wherein the calcined body having the first film is brought into contact with a solution containing a metal alkoxide, and the alkoxide is hydrolyzed and polycondensed to form the second layer.
5. The method for producing a nitride fluorescent material according to claim 4 , wherein the metal alkoxide is tetraethoxysilane.
6. The method for producing a nitride fluorescent material according to claim 1 , wherein the second heat treatment temperature is in a range of 300° C. or higher and 400° C. or lower.
7. The method for producing a nitride fluorescent material according to claim 1 , wherein the fluorescent material core has a composition represented by the following formula (I):
M a v M b w M c x Al 3-y Si y N z (I)
wherein M a represents at least one element selected from the group consisting of Sr, Ca, Ba and Mg, M b represents at least one element selected from the group consisting of Li, Na and K, M c represents at least one element selected from the group consisting of Eu, Ce, Tb and Mn, v, w, x, y and z each independently represent a number satisfying 0.80≤v≤1.05, 0.80≤w≤1.05, 0.001<x≤0.1, 0≤y≤0.5, and 3.0≤z≤5.0.