CN110386820B - Aluminum oxynitride matrix fluorescent ceramic and preparation method thereof - Google Patents
Aluminum oxynitride matrix fluorescent ceramic and preparation method thereof Download PDFInfo
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Abstract
The invention provides a complex phase fluorescent ceramic which comprises an aluminum oxynitride phase serving as a matrix phase, fluorescent powder uniformly distributed in the matrix phase and an aluminum oxide phase mixed with the fluorescent powder and the aluminum oxynitride phase. The preparation method of the complex phase fluorescent ceramic comprises the steps of coating a layer of aluminum oxide on the surface of fluorescent powder or aluminum oxynitride, and then carrying out composite sintering with the aluminum oxynitride or the fluorescent powder to form the complex phase fluorescent ceramic; or the complex phase fluorescent ceramic is formed by uniformly mixing aluminum oxynitride, aluminum oxide and fluorescent powder, ball-milling and then sintering together. The multiphase fluorescent ceramic provided by the invention is a fluorescent ceramic with high luminous efficiency, high thermal conductivity, excellent thermal shock resistance and excellent mechanical strength, and can be excited by a high-power excitation light source to realize a high-brightness semiconductor light source, such as a high-power white light LED light source, a blue light laser light source and the like.
Description
Technical Field
The invention relates to a fluorescent ceramic of an aluminum oxynitride matrix and a preparation method thereof.
Background
At present, the high-power white light LED light source is mainly implemented by the following methods: one way is to coat the LED semiconductor chip with a transparent ceramic. In order to obtain a suitable color temperature, the material of the transparent light-emitting body is generally thick (150 μm or more), and this scheme mainly has a problem that the transparent ceramic light-emitting body emits light in a bulk phase, which is different from a powder phase and a liquid phase, and the light-emitting body emits light, and the light is easily emitted from the side, which results in a reduction in the collection efficiency of the light-receiving lens. In order to improve the light receiving efficiency, the second mode is to use the translucent fluorescent ceramic with reduced thickness, and for the high color temperature product, the translucent fluorescent ceramic needs to be reduced to be less than 100 μm in thickness. However, when the thickness is reduced to less than 100 μm, the mechanical strength of the translucent fluorescent ceramic is poor, the ceramic is brittle, the yield is low, and the packaging difficulty is high in mass production.
On the other hand, for the mode of exciting the fluorescent ceramic to emit light by using the blue laser light source, the on-off response of the semiconductor light source is in the nanosecond order due to the high brightness characteristic of the blue laser, and the extremely fast response characteristic has extremely high thermal shock to the fluorescent ceramic, so that the requirements on the thermal conductivity and the thermal shock resistance of the fluorescent ceramic are high. Further, for the remote rotating laser fluorescent light source technology, there is a higher demand for the mechanical strength of the fluorescent ceramic wheel with large size rotating at high speed.
Therefore, for the development of high-brightness semiconductor light sources, high luminous efficiency and high thermal conductivity of translucent fluorescent ceramics are required, and at the same time, excellent thermal shock resistance and mechanical strength are required.
It should be noted that there are two main implementations of the translucent luminescent ceramic: one way is to add pores in the single-phase luminescent ceramic; the second method is a method using complex phase ceramics, as shown in fig. 1, which includes a complex phase ceramic matrix phase 1-1 and a phosphor phase 1-2. The main heterogeneous ceramic at present is alumina (Al)2O3) A matrix fluorescent ceramic (e.g., patent CN107285745A) and an aluminum nitride (AlN) matrix fluorescent ceramic (e.g., patent CN 107200587A). For ultra-thin (thickness of100 μm or less), both of which have a low mechanical strength and a poor thermal shock resistance, although they have a high thermal conductivity.
Therefore, it is desired to provide a complex phase ceramic having high luminous efficiency, high thermal conductivity, excellent thermal shock resistance, and excellent mechanical strength.
Disclosure of Invention
In view of the above, the present invention aims to provide a novel multiphase fluorescent ceramic, wherein Ce is added to YAG3+Adding aluminum oxide (Al) between/AlON composite phase ceramics2O3) Thereby realizing a novel YAG Ce3+/Al2O3The complex phase fluorescent ceramic with the structure of/AlON. Meanwhile, the invention also aims to provide a preparation method of the complex phase fluorescent ceramic so as to prepare the novel complex phase fluorescent ceramic.
According to an aspect of the present invention, there is provided a complex phase fluorescent ceramic including an aluminum oxynitride phase as a matrix phase, a phosphor uniformly distributed in the matrix phase, and an alumina phase mixed with the phosphor and the aluminum oxynitride phase.
Further, the phosphor and the aluminum oxynitride phase are separated from each other via the alumina phase.
Further, the alumina phase is coated on the surface of the phosphor or the aluminum oxynitride phase.
Further, the fluorescent powder is YAG Ce fluorescent powder or LuAG Ce fluorescent powder.
Further, the thickness of the alumina phase is 0.05-5 μm.
Further, the fluorescent powder accounts for 20-80% of the total volume of the complex phase fluorescent ceramic.
Further, the aluminum oxynitride phase may further include an active ion Mn2+。
According to another aspect of the present invention, there is provided a method for preparing a complex phase fluorescent ceramic, the method comprising the steps of: s1: coating a layer of aluminum oxide on the surface of the fluorescent powder or the aluminum oxynitride powder, wherein the particle size of the fluorescent powder is 5-30 mu m, and the particle size of the aluminum oxynitride powder is 0.05-1 mu m; s2: uniformly mixing and ball-milling the coated product prepared in the step S1 with aluminum oxynitride powder or fluorescent powder, an auxiliary agent and a solvent to prepare mixed slurry containing the raw materials; s3: drying and dry-pressing the mixed slurry prepared in the step S2, then performing isostatic pressing to obtain a biscuit, and performing degreasing treatment on the biscuit to obtain a ceramic body; s4: and sintering the ceramic blank prepared in the step S3 to obtain the complex phase fluorescent ceramic containing the fluorescent powder, the alumina phase and the aluminum oxynitride phase.
Further, the method for preparing the complex phase fluorescent ceramic according to the present invention further includes step S5 after step S4: and (4) carrying out post-treatment on the complex phase fluorescent ceramic prepared in the S4, wherein the post-treatment comprises thinning treatment and polishing treatment.
Further, in S1, coating a layer of aluminum oxide on the surface of the phosphor or aluminum oxynitride powder is achieved by the following method: the method comprises the steps of coating a layer of aluminum salt on the surface of fluorescent powder or aluminum oxynitride powder by adopting a coprecipitation method, and then carrying out heat treatment on the fluorescent powder or aluminum oxynitride powder coated with the aluminum salt to obtain the fluorescent powder or aluminum oxynitride powder coated with a layer of aluminum oxide on the surface.
Advantageous effects
In the complex phase fluorescent ceramic according to the present invention and the complex phase fluorescent ceramic prepared by the method for preparing the complex phase fluorescent ceramic according to the present invention, since alumina (Al) is used2O3) And phosphor (YAG: Ce)3+) And has better compatibility with aluminum oxynitride (AlON), so that Al2O3The addition of (A) greatly improves the YAG to Ce ratio3+Sintering compactness of/AlON complex phase fluorescent ceramic and Al simultaneously2O3The refractive index of the fluorescent ceramic is 1.72, which is obviously lower than the refractive index of YAG (yttrium aluminum garnet) 1.83 and the refractive index of AlON (aluminum oxynitride) 1.80, the reflectivity between different phase interfaces is improved by utilizing the refractive index difference, the light transmittance of the fluorescent ceramic is reduced, and the light efficiency is improved. Further, YAG: Ce3+/Al2O3Translucent fluorescent ceramic with AlON structure and high thermal conductivityThe high-efficiency high-performance light-emitting diode has high light efficiency, high mechanical strength and high thermal shock resistance when being processed to the thickness of less than 100 mu m. Therefore, the complex phase fluorescent ceramic can emit high-power excited light, realize higher processing yield and easier mass production packaging, can be excited by a high-power excitation light source (such as blue light laser, blue light LED and other excitation light sources), and realize high-brightness semiconductor light sources, such as high-power white light LED light sources, blue light laser light sources and the like.
Drawings
The drawings represent non-limiting exemplary embodiments described herein. It will be appreciated by those skilled in the art that the components in the figures are not necessarily to scale, emphasis instead being placed upon illustrating the principles of the invention. In the drawings:
FIG. 1 is a schematic representation of a complex phase fluorescent ceramic according to the prior art.
FIG. 2 is a schematic view of a complex phase fluorescent ceramic according to the present invention.
FIG. 3 is a flow chart of a method for preparing the complex phase fluorescent ceramic according to example 1 of the present invention.
FIG. 4 is a flow chart of a method for preparing a complex phase fluorescent ceramic according to example 2 of the present invention.
FIG. 5 is a flow chart of a method for preparing a complex phase fluorescent ceramic according to example 3 of the present invention.
List of reference numerals
1-1: multiple phase ceramic matrix phase
1-2: YAG Ce or LuAG Ce fluorescent powder
1: fluorescent powder
2: alumina phase
3: aluminum oxynitride phase
Detailed Description
One or more exemplary embodiments of the present invention are described more fully hereinafter with reference to the accompanying drawings, in which one or more exemplary embodiments of the invention can be readily ascertained by one skilled in the art. As those skilled in the art will recognize, the exemplary embodiments may be modified in various different ways without departing from the spirit or scope of the present invention, which is not limited to the exemplary embodiments described herein.
Embodiments of the present invention will now be described in detail with reference to the accompanying drawings.
The invention provides a high-strength semitransparent complex phase fluorescent ceramic, as shown in figure 2, the complex phase fluorescent ceramic comprises fluorescent powder 1, an alumina phase 2 and an aluminum oxynitride phase 3. The aluminum oxynitride phase 3 is a matrix phase, and the fluorescent powder 1 is uniformly distributed in the matrix phase. The alumina phase 2 may be mixed with the phosphor 1 and the aluminum oxynitride phase 3. Specifically, the alumina phase 2 may be coated on the surface of the phosphor 1. Alternatively, the alumina phase 2 may be coated on the surface of the aluminum oxynitride phase 3. In other words, the phosphor 1 and the aluminum oxynitride phase 3 may be separated from each other via the alumina phase 2. That is, the alumina phase 2 may be combined in contact with the phosphor 1 and the aluminum oxynitride phase 3, respectively, at the phase interfaces. Alternatively, the phosphor may be a phosphor such as YAG Ce or LuAG Ce, and the particle size of the phosphor may be 5 to 30 μm. The phosphor is formed by composite sintering of a surface alumina phase and an aluminum oxynitride phase, and the complex phase phosphor ceramic containing the aluminum oxynitride phase, the alumina phase and the phosphor is formed, wherein the thickness of the alumina phase on the surface of the phosphor can be 0.05-5 μm to fully coat the phosphor and have good light transmittance, and in order to enable the obtained complex phase phosphor ceramic to have good luminous efficiency, the phosphor can account for 20-80% of the total volume of the complex phase phosphor ceramic. When the YAG Ce or LuAG Ce is used as the fluorescent powder, the structure of the complex phase fluorescent ceramic is YAG Ce/Al2O3Ce/Al/AlON or LuAG2O3AlON, the luminescent phase is YAG to Ce or LuAG to Ce, and the matrix phase is Al2O3And AlON.
In the complex phase fluorescent ceramic of the present invention, alumina (Al)2O3) The addition of (A) can eliminate the phase interface between the phosphor powder (YAG: Ce) and aluminum oxynitride (AlON) with poor compatibility in the prior art, and replace Al with the phosphor powder (YAG: Ce) and the aluminum oxynitride (AlON)2O3Ce and YAG, and Al2O3And AlON.Due to Al2O3The ceramic material has better compatibility with YAG, Ce and AlON, so that the sintering density of the phase interface in the complex phase fluorescent ceramic is greatly improved compared with the complex phase fluorescent ceramic in the prior art. That is, the mechanical strength of the complex phase fluorescent ceramic of the present invention is greatly improved compared to the complex phase fluorescent ceramic of the prior art. In addition, Al2O3The refractive index of the ceramic is 1.72, which is obviously lower than the refractive index of YAG (yttrium aluminum garnet) 1.83 and the refractive index of AlON (aluminum oxynitride) 1.80, the reflectivity between different phase interfaces can be improved by utilizing the refractive index difference, the light transmittance of the fluorescent ceramic is reduced, and the light effect is improved, so that the luminous efficiency of the complex phase fluorescent ceramic can be improved. At the same time, Al2O3Is also high in thermal conductivity, so that Al2O3The addition of the (B) improves the heat-conducting property of the complex phase fluorescent ceramic. Further, due to the existence of AlON, the complex phase fluorescent ceramic has extremely high mechanical strength and thermal shock resistance.
Compared with the prior art, the multiphase fluorescent ceramic has high thermal conductivity, still has higher luminous efficiency, higher mechanical strength and higher thermal shock resistance when being processed to the thickness of less than 100 mu m, can be excited by a high-power blue light source, and realizes high-brightness semiconductor light sources, such as a high-power white light LED light source, a blue light laser light source and the like.
Further, the above-mentioned complex phase fluorescent ceramic in the present invention can be prepared by a preparation method comprising the following steps.
S1: the surface of the fluorescent powder or the aluminum oxynitride powder is coated with a layer of aluminum oxide, the particle size of the fluorescent powder is 5-30 mu m, and the particle size of the aluminum oxynitride powder is 0.05-1 mu m. Specifically, a coprecipitation method is adopted to coat a layer of aluminum salt on the surface of the fluorescent powder or the aluminum oxynitride powder, and the fluorescent powder or the aluminum oxynitride powder with a layer of aluminum oxide coated on the surface is obtained after heat treatment.
S2: and (3) uniformly mixing and ball-milling the coated product prepared in the step (S1) with aluminum oxynitride powder or fluorescent powder, an auxiliary agent and a solvent to prepare mixed slurry containing the raw materials. In particular toUniformly mixing and ball-milling the phosphor (or aluminum oxynitride) coated with a layer of aluminum oxide on the surface, the aluminum oxynitride (or phosphor), the assistant and the solvent prepared in the step S1 to prepare mixed slurry containing the phosphor (or aluminum oxynitride) coated with a layer of aluminum oxide, the aluminum oxynitride (or phosphor), the assistant and the solvent, wherein the assistant may include a sintering assistant, a dispersing agent and the like, and the sintering assistant may be Y2O3Or MgO, the particle size of the sintering aid can be 0.02-1 μm, and the sintering aid accounts for 0.01-4% of the total mass of the phosphor (or aluminum oxynitride) coated with a layer of aluminum oxide, the aluminum oxynitride (or phosphor) and the sintering aid, thereby being beneficial to achieving a good sintering effect.
S3: the mixed slurry prepared in S2 is dried and dry-pressed to shape, and then a biscuit is obtained by isostatic pressing, and the biscuit is subjected to degreasing treatment to obtain a ceramic body. Specifically, the mixed slurry containing the phosphor (or aluminum oxynitride) coated with a layer of aluminum oxide, the aluminum oxynitride (or phosphor), the assistant and the solvent, which is prepared in the step S2, is placed in an oven for drying, and is subjected to dry pressing under a dry pressure of 10-20 MPa, and then an isostatic pressing under an isostatic pressure of 200-300 MPa to obtain a biscuit, and the biscuit is subjected to degreasing treatment to obtain a ceramic body, wherein the degreasing temperature of the biscuit can be 500-1000 ℃, and the degreasing time can be 2-6 hours.
S4: and sintering the ceramic blank prepared in the step S3 to obtain the complex phase fluorescent ceramic containing the fluorescent powder, the alumina phase and the aluminum oxynitride phase. Specifically, the ceramic blank prepared in S3 is placed in a sintering furnace to be sintered, and after sintering, the ceramic blank is cooled to obtain the complex phase fluorescent ceramic containing the phosphor, the alumina phase and the aluminum oxynitride phase, wherein the sintering mode may be hot pressing, air pressure, vacuum, hot isostatic pressing, or spark plasma.
S5: and (4) carrying out post-treatment on the complex phase fluorescent ceramic prepared in the S4, wherein the post-treatment comprises thinning treatment and polishing treatment.
In this way, by coating a layer of aluminum oxide on the surface of the phosphor (or aluminum oxynitride), and then mixing and sintering the phosphor (or aluminum oxynitride) coated with aluminum oxide with aluminum oxynitride (or phosphor), it can be ensured that the aluminum oxide phase is interposed between the phosphor and the aluminum oxynitride phase and the phosphor and the aluminum oxynitride phase are not in direct contact with each other. That is, the phosphor is combined with an aluminum oxide phase such as aluminum oxynitride. In other words, during sintering, phase interfaces exist only between the alumina phase and the phosphor and between the alumina phase and the aluminum oxynitride phase, while phase interfaces do not exist between the phosphor and the aluminum oxynitride phase. Because the aluminum oxide has good compatibility with the fluorescent powder and the aluminum oxynitride, the aluminum oxide can be sintered compactly, and the complex phase ceramic with higher mechanical strength is obtained. In other words, the problems that aluminum oxynitride has poor compatibility with fluorescent powder and is difficult to sinter and compact are solved. In addition, as described above, the refractive index of the aluminum oxide is significantly different from the refractive indexes of the phosphor and the aluminum oxynitride, so that the reflectivity of the phase interface between the aluminum oxide and the phosphor and the phase interface between the aluminum oxide and the aluminum oxynitride can be improved, the light transmittance of the fluorescent ceramic is reduced, and the luminous efficacy is improved. Meanwhile, the thermal conductivity of the alumina is higher, so that the heat conduction performance of the complex phase fluorescent ceramic is improved by adding the alumina. In addition, the mechanical strength and the thermal shock resistance of the aluminum oxynitride are high, so that the good mechanical strength and the good thermal shock resistance of the ultrathin fluorescent ceramic are ensured. Therefore, the luminescent ceramic with high luminous efficiency, high thermal conductivity, excellent thermal shock resistance and excellent mechanical strength is prepared, has high sintering density and high light conversion efficiency, can be used for LED packaging, and solves the problems of poor reliability, low luminous efficiency, low processing yield and the like of the existing LED stage lamp light source.
The present invention will be described in detail below with reference to specific examples.
Example 1
FIG. 3 is a flow chart showing a method for preparing the complex phase fluorescent ceramic according to example 1 of the present invention. In this embodiment, high-purity aluminum oxynitride is used as a matrix phase material, commercial YAG: Ce phosphor is used as a luminescent phase material, polyvinyl butyral (PVB) is used as a binder, and a dispersant, a sintering aid, and the like can be added to prepare the complex phase fluorescent ceramic. The preparation method is as follows.
First, a first step S1 is performed to coat the surface of the YAG: Ce phosphor with a layer of alumina: coating a layer of aluminum salt on the surface of the commercial YAG/Ce fluorescent powder by adopting a coprecipitation method to obtain the YAG/Ce fluorescent powder coated with the aluminum salt on the surface. Specifically, appropriate amount of commercial YAG Ce phosphor powder with particle size of 5-30 μm and aluminum nitrate (AlNO)3) Dispersing in solution (preferably anhydrous alcohol), adding precipitant (such as ammonia water or ammonium salt (such as ammonium bicarbonate) under stirring, and reacting to obtain YAG: Ce phosphor suspension coated with aluminum salt (i.e. aluminum hydroxide); and cleaning the suspension of the YAG Ce phosphor powder coated with a layer of aluminum salt by using deionized water until the pH is neutral, drying, and performing heat treatment at 300-600 ℃ to obtain YAG Ce phosphor powder particles coated with a layer of aluminum oxide. It is noted that although aluminum nitrate (AlNO) is used herein3) The surface of the YAG: Ce phosphor is coated with a layer of aluminum salt as a raw material and ammonia water or ammonium salt is used as a precipitant, but the invention is not limited thereto, and a person skilled in the art can select any suitable aluminum-containing compound as a raw material and select a suitable deposition agent according to the kind of the selected aluminum-containing compound raw material to achieve the purpose of coating the surface of the YAG: Ce phosphor with a layer of aluminum salt. Illustratively, in other embodiments, sodium metaaluminate (NaAlO) may be selected2) As a raw material, dilute hydrochloric acid (HCl) is used as a precipitator to coat a layer of aluminum salt (namely, aluminum hydroxide) on the surface of YAG: Ce fluorescent powder. In addition, although the surface of the YAG: Ce phosphor is coated with a layer of aluminum salt by the coprecipitation method, the present invention is not limited thereto, and any method of coating the surface of the YAG: Ce phosphor with a layer of aluminum salt may be used, for example, spray drying method. It is to be understood that aluminum salts are defined herein in the broadest sense as aluminum-containing compounds, including, for example, aluminum hydroxide (Al (OH)3) Aluminum nitrate (AlNO)3) Aluminum sulfate (Al)2(SO4)3) And sodium metaaluminate (NaAlO)2) And potassium metaaluminate (KAlO)2) And the like meta-aluminates.
Then, a second step S2 is performed to mix: aluminum oxynitride powder with the grain size of 0.05-5 mu m, YAG (yttrium aluminum garnet) obtained in S1 and coated with a layer of aluminum oxide, Ce fluorescent powder, solvent and sintering aid Y with the grain size of 0.02-1 mu m2O3Or MgO is uniformly mixed and ball-milled for 6-24 hours to prepare mixed slurry of aluminum oxynitride and the YAG and Ce fluorescent powder coated with a layer of aluminum oxide, wherein the sintering aid accounts for 0.01-4% of the total mass of the aluminum oxynitride, the YAG and Ce fluorescent powder coated with a layer of aluminum oxide and the sintering aid.
Next, a third step S3 is performed to perform biscuit molding: and (3) drying the mixed slurry obtained in the step (S2) in an oven, grinding and sieving to avoid powder agglomeration to generate adverse effects on ceramic sintering, carrying out dry pressing molding under the dry pressing pressure of 10-20 MPa, carrying out isostatic pressing under the isostatic pressing pressure of 200-300 MPa to obtain a biscuit, and carrying out degreasing treatment on the biscuit to obtain a ceramic blank, wherein the degreasing temperature of the biscuit is 500-1000 ℃, and the degreasing time is 2-5 h.
Next, a fourth step S4 is performed to perform ceramic sintering: sintering the ceramic blank obtained in the step S3 under the sintering pressure of 20-80 MPa and the sintering temperature of about 1600-2000 ℃ in a hot-pressing sintering mode, and then annealing the sintered ceramic in a nitrogen atmosphere to obtain the complex phase fluorescent ceramic containing the fluorescent powder, the alumina phase and the nitrogen-alumina phase and having the structure shown in figure 2.
Finally, a fifth step S5 is executed to perform ceramic post-processing: and (4) carrying out post-treatment including thinning and polishing treatment on the complex-phase fluorescent ceramic obtained in the S4.
In the embodiment, the thickness of the aluminum oxide coated on the surface of the obtained YAG: Ce fluorescent powder is 0.05-5 μm, so that the fluorescent powder can be completely coated and the light transmittance is good. It can be understood that, when the thickness of the alumina is relatively thin, the alumina phase may not be able to completely coat the phosphor, and the aluminum oxynitride phase may be in direct contact with the phosphor, resulting in poor sintering density of the prepared complex phase phosphor ceramic. It can also be understood that when the thickness of the aluminum oxide is thicker, the light transmittance is reduced, which affects the light extraction efficiency of the phosphor. Therefore, it is important to prepare alumina of a suitable thickness for the present invention. The thickness of the alumina phase coated on the surface of the phosphor can be controlled by adjusting the concentration of the precipitation solution, or by repeating the precipitation and sintering processes (i.e., the alumina coating process) in S1 a plurality of times. For example, the first step S1 can be performed by dispersing appropriate amounts of commercial YAG: Ce phosphor having a particle size of 5 to 30 μm and aluminum nitrate in a solution (preferably absolute ethanol) to obtain an alumina phase with a desired thickness, adding a precipitant, which can be ammonia or an ammonium salt (such as ammonium bicarbonate), while stirring, and reacting sufficiently to obtain a suspension of YAG: Ce phosphor coated with a layer of aluminum salt (i.e., aluminum hydroxide); washing the suspension of YAG and Ce fluorescent powder coated with a layer of aluminum salt by using deionized water until the pH is neutral, drying, and performing heat treatment at 300-600 ℃ to obtain YAG and Ce fluorescent powder coated with a layer of aluminum oxide; then, the YAG/Ce phosphor coated with a layer of alumina and aluminum nitrate are dispersed in a solution (preferably absolute ethyl alcohol) again, a precipitator is added while stirring, after full reaction, a layer of aluminum salt (namely aluminum hydroxide) is coated again on the basis of the alumina layer of the YAG/Ce phosphor, and the YAG/Ce phosphor coated with more alumina is obtained after heat treatment at 300-600 ℃. It should be noted that although the alumina coating process is repeated once by way of example, it may be repeated a plurality of times depending on the concentration of the precipitant used, thereby obtaining an alumina phase of a desired thickness.
In the embodiment, a layer of aluminum oxide is coated on the surface of the YAG/Ce fluorescent powder, and then the aluminum oxide powder and the YAG/Ce fluorescent powder are mixed and sintered together, so that the direct contact between the YAG/Ce fluorescent powder with poor compatibility and the aluminum oxide powder can be avoided, the aluminum oxide is arranged between the YAG/Ce fluorescent powder and the aluminum oxide powder, and the aluminum oxide powder are sintered and compacted in the sintering process, the problem of poor sintering compactness of the YAG/Ce fluorescent powder and the aluminum oxide powder is solved, and the complex phase fluorescent ceramic with improved mechanical strength is obtained.
Example 2
FIG. 4 is a flow chart showing a method for preparing the complex phase fluorescent ceramic according to example 2 of the present invention. In this example, as in example 1, high-purity aluminum oxynitride was used as a matrix phase material, commercial YAG: Ce phosphor was used as a luminescent phase material, polyvinyl butyral (PVB) was used as a binder, and a dispersant, a sintering aid, and the like were added to prepare the complex phase fluorescent ceramic. The preparation method is as follows.
First, a first step S1 is performed to coat the surface of the YAG: Ce phosphor with a layer of alumina, unlike the embodiment 1 in which the surface of the aluminum oxynitride powder is coated with a layer of alumina: the same coprecipitation method as in example 1 was used to coat a layer of aluminum salt on the surface of the aluminum oxynitride powder to obtain an aluminum oxynitride powder coated with a layer of aluminum salt on the surface. Specifically, a proper amount of aluminum oxynitride powder with the particle size of 0.05-1 mu m and aluminum nitrate (AlNO)3) Dispersing in solution (preferably anhydrous ethanol), adding precipitant (such as ammonia water or ammonium salt (such as ammonium bicarbonate) under stirring, and reacting to obtain suspension of aluminum oxynitride powder coated with aluminum salt (i.e. aluminum hydroxide); the suspension of the aluminum oxynitride powder coated with the aluminum salt is washed with deionized water until the pH value is neutral and dried, and the aluminum oxynitride powder coated with the aluminum oxide layer on the surface is obtained after heat treatment at 300-600 ℃, wherein the particle size of the aluminum oxynitride powder is 0.05-1 μm, is smaller than the particle size of commercial fluorescent powder by 5-30 μm, and has a larger specific surface area, so that compared with the case of coating the aluminum oxide layer on the surface of the fluorescent powder in example 1, the feasibility of coating the aluminum oxide layer on the surface of the aluminum oxynitride powder is higher. In this embodiment, as in embodiment 1, any suitable aluminum-containing compound may be selected as a raw material, and a suitable deposition agent may be selected depending on the kind of the selected aluminum-containing compound raw material for the purpose of coating the surface of the aluminum oxynitride powder with a layer of aluminum salt. Also, the same as in embodiment 1, except that it is possible to use in this embodimentThe aluminum oxynitride powder may be coated with a layer of aluminum salt by any method other than the coprecipitation method, such as a spray drying method, in which the surface of the aluminum oxynitride powder is coated with a layer of aluminum salt.
Then, a second step S2 is performed to mix: coating the aluminum oxynitride powder obtained in S1 with a layer of aluminum oxide on the surface, commercial YAG Ce fluorescent powder with the particle size of 5-30 mu m, solvent and sintering aid Y with the particle size of 0.02-1 mu m2O3Or MgO is uniformly mixed and ball-milled for 6-24 hours to prepare the mixed slurry of aluminum oxynitride with a layer of aluminum oxide coated on the surface and YAG and Ce fluorescent powder, wherein the sintering aid accounts for 0.01-4% of the total mass of the aluminum oxynitride with a layer of aluminum oxide coated on the surface, the YAG and Ce fluorescent powder and the sintering aid.
Next, a third step S3 is performed to perform biscuit molding: and (3) drying the mixed slurry obtained in the step (S2) in an oven, grinding and sieving to avoid powder agglomeration to generate adverse effects on ceramic sintering, carrying out dry pressing molding under the dry pressing pressure of 10-20 MPa, carrying out isostatic pressing under the isostatic pressing pressure of 200-300 MPa to obtain a biscuit, and carrying out degreasing treatment on the biscuit to obtain a ceramic blank, wherein the degreasing temperature of the biscuit is 500-1000 ℃, and the degreasing time is 2-5 h.
Next, a fourth step S4 is performed to perform ceramic sintering: sintering the ceramic blank obtained in the step S3 under the sintering pressure of 20-80 MPa and the sintering temperature of about 1600-2000 ℃ in a hot-pressing sintering mode, and then annealing the sintered ceramic in a nitrogen atmosphere to obtain the complex phase fluorescent ceramic which has the structure shown in figure 2 and contains fluorescent powder, an alumina phase and an aluminum oxynitride phase.
Finally, a fifth step S5 is executed to perform ceramic post-processing: the complex phase fluorescent ceramic obtained in S4 is subjected to post-treatment including thinning and polishing treatments.
Also, in the present embodiment, the thickness of the aluminum oxide coated on the surface of the aluminum oxynitride powder obtained is 0.05 to 5 μm, so that the aluminum oxynitride powder can be completely coated and has good light transmittance. As in example 1, the thickness of the alumina phase coated on the surface of the aluminum oxynitride powder can be controlled by adjusting the concentration of the precipitation solution or repeating the precipitation and sintering process (i.e., the alumina coating process) in S1 a plurality of times.
In the embodiment, a layer of aluminum oxide is coated on the surface of the aluminum oxynitride powder, and then the aluminum oxide and the YAG and Ce fluorescent powder are mixed and sintered together, so that the direct contact between the YAG and Ce fluorescent powder with poor compatibility and the aluminum oxynitride can be avoided, the aluminum oxide is arranged between the YAG and Ce fluorescent powder, and the aluminum oxide is sintered and compacted in the sintering process, and the problem of poor sintering compactness of the YAG and Ce fluorescent powder and the aluminum oxynitride is solved, so that the complex phase fluorescent ceramic with improved mechanical strength is obtained.
Example 3
FIG. 5 is a flow chart showing a method for preparing the complex phase fluorescent ceramic according to example 3 of the present invention. This embodiment is different from embodiment 1 and embodiment 2. In the first step S1 of this embodiment, alumina is not coated on the surface of the phosphor or the aluminum oxynitride powder, but alumina powder, aluminum oxynitride powder, commercial YAG: Ce phosphor, a solvent, and a sintering aid are directly and uniformly mixed and ball-milled for 6 to 24 hours to prepare a mixed slurry containing alumina powder, aluminum oxynitride powder, and YAG: Ce phosphor.
Then, a second step S2 is performed to perform biscuit forming: and (3) drying the mixed slurry obtained in the step (S1) in an oven, grinding and sieving to avoid powder agglomeration to generate adverse effects on ceramic sintering, carrying out dry pressing molding under the dry pressing pressure of 10-20 MPa, carrying out isostatic pressing under the isostatic pressing pressure of 200-300 MPa to obtain a biscuit, and carrying out degreasing treatment on the biscuit to obtain a ceramic blank, wherein the degreasing temperature of the biscuit is 500-1000 ℃, and the degreasing time is 2-5 h.
Next, a third step S3 is performed to perform high temperature sintering: and sintering the ceramic blank obtained in the step S2 under the sintering pressure of 20-80 MPa and the sintering temperature of about 1600-2000 ℃ in a hot-pressing sintering mode, and then annealing the sintered ceramic in a nitrogen atmosphere to obtain the complex phase fluorescent ceramic containing the fluorescent powder, the alumina phase and the nitrogen-alumina phase.
Finally, a fourth step S4 is executed to perform ceramic post-processing: and (4) carrying out post-treatment including thinning and polishing treatment on the complex-phase fluorescent ceramic obtained in the S3.
In this embodiment, unlike the embodiments 1 and 2 in which a layer of alumina is coated on the surface of the YAG: Ce phosphor or aluminum oxynitride powder, and then the coated alumina is compositely sintered with the aluminum oxynitride powder or the YAG: Ce phosphor to form the multi-phase phosphor, this coating is not performed in this embodiment, but three phases of the YAG: Ce phosphor, the alumina powder, and the aluminum oxynitride powder are uniformly mixed and sintered. The ceramic prepared by the method in the embodiment can not completely avoid direct contact between the YAG Ce fluorescent powder and the aluminum oxynitride phase, so that the strength is slightly lower than that of the ceramic prepared in the embodiments 1 and 2, but the addition of the aluminum oxide can still reduce the phase interface between the YAG Ce fluorescent powder and the aluminum oxynitride phase to a certain degree, so that the sintering density of the YAG Ce/AlON complex phase fluorescent ceramic is greatly improved, meanwhile, the preparation method of the ceramic is simpler than that of the embodiments 1 and 2, more aluminum oxide can be added in a simple manner, and the thermal conductivity of the obtained complex phase fluorescent ceramic can be higher under the condition that the content of the aluminum oxide is increased.
Example 4
In the present example, the active ion Mn was increased in the binder phase AlON used, compared to examples 1, 2 and 32+And the rest was the same as in example 1, example 2 and example 3, thereby preparing y-AlON containing Mn2+Another complex phase fluorescent ceramic of green ceramic. The multiphase fluorescent ceramic prepared in the embodiment has the advantage of supplementing YAG to Ce3+The green light is insufficient, and the color rendering index of a green light wave band is improved.
The fluorescent ceramics prepared in the above examples 1 to 4 are multiphase fluorescent ceramics, and the bonding phase is AlON and Al2O3The luminescent phase is YAG Ce fluorescent powder, the complex phase fluorescent ceramic has two structures, one structure is complex phase ceramic formed by compounding thin layer aluminum oxide (thickness is 0.05-5 mu m) coated on the surface of the fluorescent powder and aluminum oxynitrideThe ceramic can also be a complex phase ceramic compounded by aluminum oxide (0.05-5 mu m) coated on the surface of aluminum oxynitride powder and fluorescent powder; the other structure is a complex phase ceramic formed by uniformly compounding aluminum oxide powder, aluminum oxynitride powder and fluorescent powder; in addition, the aluminum oxynitride ceramic can also be gamma-AlON: Mn2+Green ceramic. The complex phase fluorescent ceramic has high luminous efficiency, high thermal conductivity, excellent thermal shock resistance and excellent mechanical strength, still has higher luminous efficiency and stronger mechanical strength and thermal shock resistance when being processed to be less than 100 mu m, can emit high-power white light, realizes higher processing yield and easier mass production packaging, can be excited by a high-power excitation light source, and realizes high-brightness semiconductor light sources, such as high-power white light LED light sources, blue light laser light sources and the like.
In the above embodiment, the particle size of the aluminum oxynitride powder is 0.05-1 μm, the particle size of the YAG-Ce phosphor is 5-30 μm, the phosphor accounts for 20-80% of the total mass of the aluminum oxynitride, the phosphor and the sintering aid, and the sintering aid is Y2O3Or MgO, the particle size of the sintering aid is 0.02-1 μm, and the sintering aid accounts for 0.01-4% of the total mass of the aluminum oxynitride, the fluorescent powder and the sintering aid.
On the other hand, the phosphor in the above embodiment can be replaced by LuAG Ce phosphor, and the structure of the prepared complex phase fluorescent ceramic is LuAG Ce-Al2O3AlON, wherein the luminescent phase is LuAG Ce fluorescent powder. The high-density sintered compact and the high light efficiency can be realized, the high-density sintered compact and the high-light efficiency sintered compact have high light efficiency, strong mechanical strength and thermal shock resistance when being processed to be less than 100 mu m, and also have high thermal conductivity, so that high-power white light can be emitted, high processing yield and easy mass production packaging can be realized, the high-power white light can be excited by a high-power blue light source, and high-brightness semiconductor light sources such as a high-power white light LED light source, a blue light laser light source and the like can be realized.
The raw materials listed in the invention, the upper and lower limits of the raw materials, the upper and lower limits of the process parameters and the values of the intervals can all realize the invention, and the examples are not listed; any simple modifications or equivalent changes made to the above embodiments according to the technical spirit of the present invention still fall within the scope of the technical solution of the present invention.
Claims (8)
1. The complex phase fluorescent ceramic is characterized by comprising an aluminum oxynitride phase serving as a matrix phase, fluorescent powder uniformly distributed in the matrix phase and an alumina phase mixed with the fluorescent powder and the aluminum oxynitride phase; the phosphor and the aluminum oxynitride phase are separated from each other by the alumina phase; the aluminum oxide phase is coated on the surface of the fluorescent powder or the aluminum oxynitride phase.
2. The complex phase fluorescent ceramic according to claim 1,
the fluorescent powder is YAG Ce fluorescent powder or LuAG Ce fluorescent powder.
3. The complex phase fluorescent ceramic according to claim 1,
the thickness of the alumina phase is 0.05-5 μm.
4. The complex phase fluorescent ceramic according to claim 1,
the fluorescent powder accounts for 20-80% of the total volume of the complex phase fluorescent ceramic.
5. The complex phase fluorescent ceramic according to claim 1,
the aluminum oxynitride phase also comprises an active ion Mn2+。
6. A method for preparing a complex phase fluorescent ceramic, the method comprising the steps of:
s1: coating a layer of aluminum oxide on the surface of the fluorescent powder or the aluminum oxynitride powder, wherein the particle size of the fluorescent powder is 5-30 mu m, and the particle size of the aluminum oxynitride powder is 0.05-1 mu m;
s2: uniformly mixing and ball-milling the coated product prepared in the step S1 with aluminum oxynitride powder or fluorescent powder, an auxiliary agent and a solvent to prepare mixed slurry containing the raw materials;
s3: drying and dry-pressing the mixed slurry prepared in the step S2, then performing isostatic pressing to obtain a biscuit, and performing degreasing treatment on the biscuit to obtain a ceramic body;
s4: and sintering the ceramic blank prepared in the step S3 to obtain the complex phase fluorescent ceramic containing the fluorescent powder, the alumina phase and the aluminum oxynitride phase.
7. The method of claim 6, further comprising, after the step S4, a step S5: and (4) carrying out post-treatment on the complex phase fluorescent ceramic prepared in the S4, wherein the post-treatment comprises thinning treatment and polishing treatment.
8. The method of claim 6,
in S1, coating a layer of aluminum oxide on the surface of the phosphor or aluminum oxynitride powder is achieved by the following method: the method comprises the steps of coating a layer of aluminum salt on the surface of fluorescent powder or aluminum oxynitride powder by adopting a coprecipitation method, and then carrying out heat treatment on the fluorescent powder or aluminum oxynitride powder coated with the aluminum salt to obtain the fluorescent powder or aluminum oxynitride powder coated with a layer of aluminum oxide on the surface.
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