CN108105604B - Luminescent ceramic structure, preparation method thereof, related light-emitting device and projection device - Google Patents
Luminescent ceramic structure, preparation method thereof, related light-emitting device and projection device Download PDFInfo
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Abstract
The invention discloses a luminescent ceramic structure, a preparation method thereof, a related light-emitting device and a projection device. The luminescent ceramic structure comprises a luminescent ceramic layer, a porous ceramic reflecting layer and an aluminum nitride ceramic radiating substrate which are sequentially laminated and combined together; wherein the porous ceramic reflective layer is an alumina porous ceramic doped with zinc oxide and/or magnesium oxide for bonding with the ceramic heat-dissipating substrate, and the doped zinc oxide and/or magnesium oxide is at least partially Zn-dopedxAlyO and/or MgxAlyO is present to enhance the adhesion to the aluminum nitride ceramic substrate. The luminescent ceramic structure has the characteristics of high thermal conductivity, strong bonding force and high reliability, and can be used as an optical device of a relevant light-emitting device and a projection device.
Description
Technical Field
The invention relates to the technical field of illumination and display, in particular to a luminescent ceramic structure, a preparation method thereof, a related light-emitting device and a projection device.
Background
The fluorescent powder is excited by utilizing light sources such as laser or LED to obtain preset monochromatic light or polychromatic light, and the fluorescent powder is a technical scheme widely applied to the fields of lighting sources, projection display and the like. The technical scheme is that laser or LED emergent light is often incident on a fluorescent powder color wheel rotating at high speed so as to realize good heat dissipation.
At present, the packaging modes of the fluorescent powder are mainly organic silica gel packaging and inorganic glass packaging, the thermal conductivity of the two packaging modes is low (below 1W/(m.K)), the thermal damage resistance temperature is not high, the tolerance temperature of the silica gel is generally below 200 ℃, and the tolerance temperature of the glass is generally below 500 ℃.
In order to solve the problems of thermal conductivity and heat resistance, those skilled in the art have further developed a fluorescent light emitting structure of a ceramic structure. In the prior art, TW201023405A discloses a light emitting structure, which includes a light emitting ceramic layer and a porous ceramic reflective layer, wherein the porous ceramic reflective layer is a porous YAG reflective layer, and the technical scheme utilizes the heat resistance and excellent mechanical properties of the ceramic structure, and is a great improvement over the technical schemes of organic silica gel packaging and inorganic glass packaging. However, in the technical scheme generated in the LED illumination period, the light intensity of the excitation light emitted by the LED is far lower than that of the laser light at present, the luminescent ceramic layer emits a large amount of heat under the irradiation of the laser light, the heat is difficult to transfer due to the porous structure of the porous ceramic reflection layer, and a heat dissipation substrate needs to be arranged on the back surface of the porous ceramic reflection layer to improve the heat dissipation.
In the prior art, the composition material of the porous ceramic reflection layer is usually different from that of the heat dissipation substrate, so that the porous ceramic reflection layer and the heat dissipation substrate are difficult to enhance the bonding force in a co-sintering manner.
Disclosure of Invention
In order to solve the technical problems in the prior art, the invention provides a luminescent ceramic structure which has the characteristics of high thermal conductivity, strong bonding force and high reliability.
According to a first aspect of the present invention, there is provided a luminescent ceramic structure comprising a luminescent ceramic layer, a porous ceramic reflective layer and a ceramic heat-dissipating substrate laminated in this order; the porous ceramic reflecting layer is alumina porous ceramic doped with zinc oxide and/or magnesium oxide, and the doped zinc oxide and/or magnesium oxide is used for being combined with the ceramic heat dissipation substrate; and at least part of the doped zinc oxide is ZnxAlyO, and at least part of the doped magnesium oxide is MgxAlyThe form of O exists; the ceramic heat dissipation substrate is an aluminum nitride ceramic substrate.
Further, Zn is contained in the above-mentionedxAlyO is in particular ZnAl2O4，MgxAlyO is in particular MgAl2O4。
Further, the porous ceramic reflective layer is doped with at least one of zirconia, titania and yttria.
Further, the proportion of the doped oxide in the porous ceramic reflecting layer is 1-10% of the total mass.
Further, the luminescent ceramic layer is Ce-doped YAG ceramic.
Further, the thickness of the luminescent ceramic layer is 0.05-1 mm, the thickness of the porous ceramic reflection layer is 0.1-2 mm, and the thickness of the ceramic heat dissipation substrate is 0.5-5 mm.
Furthermore, the surface of the luminescent ceramic layer is plated with an antireflection film, or the surface of the luminescent ceramic layer has a rough microstructure.
According to a second aspect of the present invention, there is provided a method of making a luminescent ceramic structure as in the first aspect, comprising: casting slurry respectively used for forming the porous ceramic reflecting layer and the luminescent ceramic layer is sequentially poured on the ceramic heat dissipation substrate, and then the luminescent ceramic structure is formed through lamination and sintering in sequence.
According to a third aspect of the present invention, there is provided a light emitting device comprising the light emitting ceramic structure of the first aspect, and further comprising an excitation light source for generating excitation light, the light emitting ceramic structure being located on an optical path of the excitation light.
According to a fourth aspect of the present invention, there is provided a projection system comprising the light emitting device of the third aspect and further comprising a projection imaging device.
On one hand, the luminescent ceramic structure provided by the invention utilizes the alumina porous ceramic as the reflecting layer and also as the bonding layer to bond the luminescent ceramic layer and the ceramic heat dissipation substrate, thereby realizing higher efficiency and higher reliability. On the other hand, the alumina reflecting ceramic layer is a non-compact porous structure, so that the structure can still ensure high reflectivity under the condition of a thin thickness, and the non-compact porous structure can realize the bonding of alumina ceramics and aluminum nitride ceramics with inconsistent thermal expansion coefficients. More importantly, zinc oxide and/or magnesium oxide is added into the alumina porous ceramic to react with the trace alumina layer on the surface layer of the aluminum nitride ceramic substrate to generate ZnxAlyO and/or MgxAlyAnd O, further enhancing the adhesive force with the aluminum nitride ceramic substrate.
Drawings
FIG. 1 is a schematic structural view of one embodiment of a luminescent ceramic structure of the present invention;
FIG. 2 is a schematic structural view of another embodiment of a luminescent ceramic structure of the present invention;
FIG. 3 is a schematic structural view of yet another embodiment of a luminescent ceramic structure of the present invention.
Detailed Description
The present invention will be described in further detail with reference to the following detailed description and accompanying drawings.
In the invention, the luminescent ceramic structure comprises a luminescent ceramic layer (a first layer), a porous ceramic reflecting layer (a second layer) and a ceramic heat dissipation substrate (a third layer) which are sequentially laminated and combined together, wherein the porous ceramic reflecting layer is alumina porous ceramic, and the ceramic heat dissipation substrate is an aluminum nitride ceramic substrate. According to the technical scheme, in order to improve the binding force between the porous ceramic reflecting layer and the aluminum nitride ceramic substrate, the alumina porous ceramic layer is doped with oxide. Because the surface of the aluminum nitride ceramic substrate is easy to generate a thin layer of aluminum oxide, the oxide doped in the aluminum oxide porous ceramic layer can react with the aluminum oxide layer on the surface of the aluminum nitride to generate a composite product, and the combination of the porous ceramic reflecting layer and the ceramic heat dissipation substrate is improved by utilizing the composite product. Because the porous ceramic reflecting layer is alumina porous ceramic, the alumina of the porous ceramic reflecting layer is difficult to react with the aluminum nitride or the alumina on the surface of the aluminum nitride, the invention utilizes the additionally doped oxide to participate in the reaction and becomes a connecting bridge of the porous ceramic reflecting layer and the ceramic heat dissipation substrate, which is the main inventive concept of the invention.
The individual layers of the luminescent ceramic structure of the present invention are described individually below.
< luminescent ceramic layer >
In the embodiment of the invention, the first luminescent ceramic layer functions to receive irradiation of excitation light and convert the excitation light into excited light with different wavelengths. The excitation light may be light emitted by a solid-state light source, such as LED light, laser diode light, laser light, or any other light source light disclosed before the present application. Because the luminescent ceramic layer is of a ceramic structure, the thermal stability and the heat conductivity of the luminescent ceramic layer are far superior to those of a fluorescent powder layer which takes glass or silica gel as a substrate (namely, the fluorescent powder is encapsulated in continuous glass or silica gel), the luminescent ceramic layer can bear the irradiation of high-power exciting light, and the luminescent ceramic layer can be suitable for the field of high-brightness laser fluorescent lighting/display.
The luminescent ceramic layer can be pure-phase fluorescent ceramic, in particular to various oxide ceramic, nitride ceramic or oxynitride ceramic, and luminescent centers are formed by doping trace activator elements (such as lanthanide elements) in the preparation process of the ceramic. Because the doping amount of general activator elements is small (generally less than 1%), the fluorescent ceramics are usually transparent or semitransparent luminescent ceramics, and excitation light easily and directly passes through the luminescent ceramic layer and then is emitted, so that the luminescent ceramic layer has low luminous efficiency and is more suitable for excitation light application scenes with lower power. In one embodiment of the invention, the luminescent ceramic layer is a Ce-doped YAG ceramic; in another embodiment of the present invention, the luminescent ceramic layer is a Ce-doped LuAG ceramic.
The luminescent ceramic layer may also be a composite ceramic layer having a transparent/translucent ceramic as a matrix with luminescent ceramic particles (e.g., phosphor particles) distributed within the ceramic matrix. The transparent/translucent ceramic matrix can be a variety of oxide ceramics (e.g., alumina ceramics, Y)3Al5O12Ceramics), nitride ceramics (such as aluminum nitride ceramics) or oxynitride ceramics, the ceramic matrix being operative to conduct light and heat such that excitation light is incident on the luminescent ceramic particles and stimulated light is emitted from the luminescent ceramic layer; the luminescent ceramic particles assume the main luminescent function of the luminescent ceramic layer for absorbing the excitation light and converting it into stimulated light. The grain size of the luminescent ceramic particles is larger, and the doping amount of the activator element is larger (such as 1-5%), so that the luminescent efficiency is high; and the luminescent ceramic particles are dispersed in the ceramic matrix, thereby avoiding the luminescent ceramic particles positioned at the deeper position of the luminescent ceramic layerThe condition that the fluorescent ceramic can not be irradiated by exciting light is avoided, and the condition that the pure-phase fluorescent ceramic is poisoned by the concentration of the activator element due to large integral doping amount is avoided, so that the luminous efficiency of the luminous ceramic layer is improved.
Furthermore, scattering particles can be added in the luminescent ceramic layer, so that the scattering particles are distributed in the ceramic matrix. The scattering particles have the function of enhancing the scattering of the exciting light in the luminescent ceramic layer, so that the optical path of the exciting light in the luminescent ceramic layer is increased, the light utilization rate of the exciting light is greatly improved, and the light conversion efficiency of the luminescent ceramic layer is improved. The scattering particles may be scattering particles such as alumina, yttria, zirconia, lanthana, titania, zinc oxide, barium sulfate, etc., and may be either single-material scattering particles or a combination of two or more kinds, and the scattering particles are characterized by apparent white color, ability to scatter visible light, stable material, ability to withstand high temperature, and particle size in the same order of magnitude or one order of magnitude lower than the wavelength of the excitation light. In other embodiments, the scattering particles may be replaced by air holes with the same size, and the difference between the refractive indexes of the air holes and the ceramic matrix is used for realizing total reflection so as to scatter the exciting light or the stimulated light.
The luminescent ceramic layer may also be another composite ceramic layer that differs from the composite ceramic layer described above only in the ceramic matrix. In the present embodiment, the ceramic matrix is a phase-pure fluorescent ceramic, that is, the ceramic matrix itself has an activator and can emit excited light under irradiation of excitation light. The technical scheme integrates the advantages of high luminous efficiency of the luminescent ceramic particles of the composite ceramic layer and the advantages of luminous performance of the pure-phase fluorescent ceramic, and utilizes the luminescent ceramic particles and the ceramic matrix to emit light, so that the luminous efficiency of the luminescent ceramic layer is further improved. In the luminescent ceramic layer, scattering particles or pores can also be added to enhance the internal scattering of the luminescent ceramic layer.
Typical but non-limiting selection of luminescent ceramic particlesIs a lanthanide-doped garnet luminescent ceramic, such as Ca3(Al,Sc)2Si3O12Or else an aluminate, e.g. (Gd, Tb, Y, Lu)3(Al,Ga)5O12And Y of the composite component3Mg2AlSi2O12Etc., wherein the elements separated by commas in brackets, such as (Al, Ga), mean that the ratio of Al to Ga can be chosen arbitrarily, but the total amount of the two elements in the formula corresponds to 1, for example Al0.7Ga0.3、Al0.9Ga0.1、Al0.2Ga0.8. In one embodiment of the invention, Ce doped YAG garnet is preferred, i.e. (Y)1-xCex)3Al5O12. In another embodiment of the invention, the luminescent ceramic particles are of Ce-doped LuAG garnet structure.
In one embodiment of the present invention, the thickness of the luminescent ceramic layer is 0.05 to 1mm, and if the luminescent ceramic layer is too thin, the efficiency is reduced; if the luminescent ceramic layer is too thick, the thermal resistance is too large, which is not favorable for heat dissipation.
< porous ceramic reflective layer >
In the embodiment of the invention, the second porous ceramic reflecting layer is used for scattering and reflecting stimulated light or mixed light of the stimulated light and unabsorbed exciting light. The porous ceramic reflecting layer is specifically alumina porous ceramic, and the reflection principle is that incident light is totally reflected at the interface of alumina and pores by utilizing the refractive index difference between the pores and the alumina so as to realize the reflection effect. The refractive index of alumina is generally about 1.7, and the pores are considered to be air therein, and the refractive index is about 1, and when light enters the interface between alumina and air from the inside of alumina, total reflection occurs when the incident angle is small. The reflectivity of the porous ceramic reflecting layer can be controlled by controlling the size of the pores (such as adding pore-forming agent or controlling the temperature rise rate in the preparation process) and controlling the thickness of the porous ceramic reflecting layer. The alumina porous ceramic is high temperature resistant and oxidation resistant, is suitable for a high-power luminous ceramic structure, has uniformly distributed air holes, and is beneficial to the uniform reflectivity of all parts of the reflecting layer. The metal reflecting layer in the prior art is easy to oxidize and vulcanize, and particularly has short service life in a high-temperature environment; in addition, in the prior art, white scattering particles are bonded into a layer by using an adhesive such as glass, and the technical scheme has the defects that the adhesive is sticky in the preparation process, the white scattering particles are small in particle size, easy to agglomerate and difficult to uniformly disperse, and the reflection functional material of the reflection layer is the white scattering particles, so that the reflection rate is not uniform due to the fact that the white scattering particles cannot be uniformly dispersed.
In the embodiment of the invention, the alumina porous ceramic layer is additionally doped with oxide, and part of the oxide can react with alumina at high temperature to generate new composite oxide, and the form of the composite oxide is MxAlyO, wherein M is an element of the doped oxide. In one embodiment of the present invention, the characteristic features are: doped with at least one of zinc oxide and magnesium oxide. In the case of doping with zinc oxide, the zinc oxide is at least partially ZnxAlyIn the form of O, in the case of doping with magnesium oxide, the latter is at least partially MgxAlyThe form of O exists. The doped oxide is incorporated during the preparation process in a manner mixed with the raw material of the alumina porous ceramic layer, and during the sintering process, the doped oxide partially reacts with the alumina. The aluminum oxide porous ceramic layer is directly fired on the ceramic heat dissipation substrate, the ceramic heat dissipation substrate is a prepared aluminum nitride ceramic substrate, the surface of the aluminum nitride ceramic substrate is usually oxidized to generate an aluminum oxide film, when the aluminum oxide porous ceramic layer is fired, doped oxides (such as the magnesium oxide or the zinc oxide) in the raw materials are very easy to react with the aluminum oxide film on the surface of the aluminum nitride ceramic substrate to generate composite oxides, and the composite oxides enable the aluminum oxide porous ceramic layer and the aluminum nitride ceramic heat dissipation substrate to be combined together more tightly, so that the reliability of products is improved.
In some embodiments of the invention, ZnxAlyO is in particular ZnAl2O4，MgxAlyO is in particular MgAl2O4The composite oxide is spinel structureAnd the ceramic is stable and is beneficial to the combination of the porous ceramic layer and the ceramic heat dissipation layer. The presence of the substance can be confirmed by detecting the bonding portion between the alumina porous ceramic layer and the aluminum nitride ceramic heat dissipating substrate and performing a compositional analysis and characterization. MgAl2O4The diffraction peak card of the X-ray diffraction spectrum of (1) is PDF #21-1152, ZnAl2O4The diffraction peak card of the X-ray diffraction spectrum of (1) is PDF # 05-0669.
Of course, it is to be noted that Zn of the present inventionxAlyO and MgxAlyThe elemental ratio of Zn to Al or Mg to Al in O is not particularly limited, and in practical luminescent ceramic structure products, the elemental ratio may not appear at a fixed value, but there are many possible compound forms, differing in elemental ratio among different compound forms, with the subscripts x and y intended to represent any zinc aluminum oxide or magnesium aluminum oxide that satisfies the valence balance of the compound. For example, the composite oxide may be a composite oxide of other elements such as Zn in a molar ratio2Al2O5Etc., the presence of the complex oxide can be confirmed also by elemental analysis or X-ray diffraction spectrum.
In another embodiment of the present invention, in addition to the doping with at least one of zinc oxide and magnesium oxide, at least one of zirconium oxide, titanium oxide and yttrium oxide, which are ceramic powders having a high refractive index, are further doped, and the combination with alumina having a relatively low refractive index is advantageous in increasing the reflectance thereof. In addition, the zirconia also has a toughening function, and the mechanical property of the alumina porous ceramic layer can be improved by doping the zirconia.
In the embodiment of the present invention, the proportion of the oxide doped in the porous ceramic reflective layer is 1% to 10% of the total mass. That is, when the doped oxide is only at least one of magnesium oxide or zinc oxide, the total mass of the at least one of magnesium oxide or zinc oxide accounts for 1% to 10% of the porous ceramic reflective layer; when the doped oxide further comprises at least one of zirconia, titania, and yttria, the total mass of the at least one of magnesia or zinc oxide and the at least one of zirconia, titania, and yttria comprises the porous ceramicThe mass proportion of the injection layer is 1-10%. It is worth noting that 1% to 10% represents the mass fraction of oxide doped during the preparation, without loss during the reaction, so that in the final product 1% to 10% comprises both oxide and ZnxAlyO and/or MgxAlyThe mass fraction of O after being converted to oxide is the sum of the two.
The proportion of the doped oxide should not be too low, otherwise, insufficient composite oxide will be generated, and the effect of enhancing the combination of the porous ceramic reflection layer and the ceramic heat dissipation substrate cannot be achieved. In addition, since the thermal conductivity of the doped oxide is low and the thermal expansion coefficient is deviated from that of alumina, too high doping causes low thermal conductivity and poor cofiring stability with YAG ceramics. While a doping amount corresponding to 1% to 10% of the total mass can achieve a good effect, the basic embodiment of the present invention is not limited to this mass ratio.
The aluminum oxide porous ceramic layer and the luminescent ceramic layer are connected through sintering, slurry forming the aluminum oxide porous ceramic layer and slurry forming the luminescent ceramic layer are coated on the radiating substrate in sequence to form a laminated three-layer structure of the luminescent ceramic layer, the aluminum oxide porous ceramic layer and the radiating substrate, and the aluminum oxide porous ceramic layer and the luminescent ceramic layer are firmly combined together through sintering. In addition, the alumina porous ceramic layer and the luminescent ceramic layer can be connected through an adhesive layer after being respectively formed, and the adhesive layer can be a glass adhesive layer or an organic adhesive layer (such as silica gel, epoxy resin and the like).
In one embodiment of the invention, the thickness of the porous ceramic reflecting layer is 0.1-2 mm, and if the porous ceramic reflecting layer is too thin, the reflectivity is reduced; if the porous ceramic reflecting layer is too thick, the thermal resistance is too large, which is not favorable for heat dissipation.
< ceramic Heat-dissipating substrate >
In the embodiment of the invention, the third layer of ceramic heat dissipation substrate is used for dissipating heat conducted by the reflecting layer into the air or further dissipating the heat through other heat dissipation members. The aluminum nitride ceramic substrate is selected as the ceramic heat dissipation substrate, and the aluminum nitride ceramic has excellent heat conduction performance and good mechanical performance.
In the luminescent ceramic structure, the third layer adopts the aluminum nitride ceramic substrate as the heat dissipation substrate, the surface of the third layer is bound to have oxidized aluminum oxide, and the aluminum oxide porous ceramic of the second layer is doped with at least one of zinc oxide and magnesium oxide, so that Zn is formed at the interface between the second layer and the third layerxAlyO and MgxAlyAnd O for bonding the second layer and the third layer, thereby improving the bonding force between the two layers. For the description of the composite oxide, reference may be made to the description of the porous ceramic reflective layer described above, and the description thereof will not be repeated.
In one embodiment of the present invention, the thickness of the ceramic heat dissipation substrate is 0.5 to 5 mm. If the ceramic heat dissipation substrate is too thin, the strength is too low; if the ceramic heat dissipation substrate is too thick, it is too heavy and the substrate cost is too high.
In other embodiments of the present invention, the luminescent ceramic layer is coated with an antireflection film, which may be a multilayer of alternately coated antireflection films with high refractive index films and low refractive index films, to further improve the incident light transmittance and improve the light extraction efficiency. Or the surface of the luminescent ceramic layer is provided with a rough microstructure, specifically, a saw-toothed structure can be etched on the surface of the luminescent ceramic layer to further improve the excitation efficiency and the light extraction efficiency.
Also provided in an embodiment of the present invention is a method of making a luminescent ceramic structure, comprising: casting slurry respectively used for forming the porous ceramic reflecting layer and the luminescent ceramic layer is sequentially poured on the ceramic heat dissipation substrate, and then the luminescent ceramic structure is formed through lamination and sintering in sequence.
In one embodiment of the invention, the luminescent ceramic layer is prepared from Ce-doped YAG (YAG: Ce), the porous ceramic reflective layer is prepared from zinc oxide and/or magnesium oxide doped alumina, and aluminum nitride ceramic (thermal conductivity over 80W/mK) is used as the ceramic heat sink substrate. Firstly, preparing YAG casting slurry and porous alumina casting slurry; then, pouring the porous alumina casting slurry on a ceramic heat dissipation substrate, and drying the casting belt to obtain a green sheet; continuously pouring the YAG casting slurry on the porous alumina green sheet to form a porous alumina and YAG green sheet layer stacked on the ceramic heat dissipation substrate; and finally, obtaining a finished product of the luminescent ceramic structure through lamination and sintering.
In the embodiment, the YAG ceramic has high thermal conductivity (14W/m/K at 20 ℃ and 10.5W/m/K at 100 ℃) and high YAG melting point (1970 ℃), so that the heat dissipation efficiency and thermal damage resistance temperature of the fluorescent powder package can be greatly improved, and the application of a high-power blue LED (light-emitting diode), especially a blue laser, is met.
In the embodiment, the reflecting layer is made of porous alumina ceramic co-fired with the YAG ceramic layer, so that better reflectivity can be ensured, the thermal conductivity of the reflecting layer is higher than that of glass ceramic, and the interface thermal resistance of the co-fired manner is lower. In addition, the light-emitting ceramic structure co-fired by the reflective ceramic and the light-emitting ceramic is manufactured on the ceramic heat dissipation substrate by adopting a tape casting method, various shapes such as a square shape or a circular shape can be realized, and the tape casting thickness can be controlled, so that the structure with controllable thickness of the light-emitting layer and the reflective layer can be realized, and compared with a manufacturing method of independently manufacturing the light-emitting ceramic layer, then cutting, thinning, polishing, plating the reflective layer and welding the reflective layer on the heat conduction substrate, the process provided by the invention can be formed by one-step sintering, is simpler in process, and can realize the manufacture of a large-diameter light-emitting ceramic structure. Therefore, the method is a mass production preparation method with low cost and high efficiency.
The embodiment of the invention further provides a light-emitting device, which comprises the light-emitting ceramic structure of the embodiment of the invention and an excitation light source for generating excitation light, wherein the light-emitting ceramic structure is positioned on the light path of the excitation light. The light-emitting ceramic layer is used for absorbing exciting light to generate excited light, the porous ceramic reflecting layer is used for scattering and reflecting the excited light or mixed light of the excited light and the unabsorbed exciting light, and the ceramic heat dissipation substrate is used for dissipating heat conducted by the reflecting layer. The light-emitting device can be applied to general illumination, such as various lamps, namely street lamps, searchlights, stage lamps and automobile headlamps, and can also be applied to display systems, such as projectors, televisions and the like. The light emitting device has the advantages of energy saving (the electroluminescent light source is LD), high brightness and long service life.
The embodiment of the invention further provides a projection system, which comprises the light-emitting device of the embodiment of the invention and a projection imaging device. After the projection system adopts the light-emitting device, the maximum brightness of emergent light is obviously improved, and the projection system can be used for household miniature projection, living room projection, engineering projection and cinema projection. And the improvement of the brightness is also beneficial to the improvement of the contrast of the projector.
The technical solutions of the present invention are described in detail by the following specific examples, and it should be understood that these examples are only illustrative and should not be construed as limiting the scope of the present invention.
Example one
As shown in fig. 1, the luminescent ceramic structure of the present embodiment includes: a luminescent ceramic layer 110, a porous ceramic reflective layer 120, and a ceramic heat-dissipating substrate 130, which are sequentially laminated together; the luminescent ceramic layer 110 comprises fluorescent crystal grains 111 and a scattering medium 112, and the porous ceramic reflecting layer 120 comprises alumina porous ceramic 122 doped with zinc oxide 121; the ceramic heat dissipation substrate 130 is an aluminum nitride ceramic substrate. In the process of preparing the luminescent ceramic structure, since the surface of the aluminum nitride ceramic substrate must have oxidized aluminum oxide, and the porous ceramic reflective layer 120 is doped with zinc oxide, Zn is formedxAlyO, thereby improving the bonding force between the porous ceramic reflective layer 120 and the ceramic heat dissipation substrate 130.
The luminescent ceramic structure of the embodiment is prepared by a tape casting method, and specifically includes the following steps:
preparation of YAG casting slurry: firstly, mixing synthetic raw materials of yttrium oxide, aluminum oxide, cerium oxide and a fluxing agent TEOS (tetraethyl orthosilicate) and adding the mixture into an ethanol solvent, and then ball-milling the mixture for a period of time by using aluminum oxide balls. The ball-milled slurry is mixed with a polymeric binder such as, but not limited to, polyvinyl butyral (PVB), and a plasticizer such as, but not limited to, Benzyl Butyl Phthalate (BBP), polyethylene glycol (PEG). The binder and the plasticizer may be directly added and mixed with the slurry, or dissolved in a solvent in advance and then added to the slurry.
2. Preparing porous alumina casting slurry: firstly, synthetic raw materials of alumina, doped zinc oxide and a pore-forming agent are mixed and added into an ethanol solvent, wherein the pore-forming agent can be starch or PMMA microspheres (polymethyl methacrylate), and then alumina balls are used for ball milling for a period of time. The ball-milled slurry is mixed with a polymeric binder such as, but not limited to, polyvinyl butyral (PVB), and a plasticizer such as, but not limited to, Benzyl Butyl Phthalate (BBP), polyethylene glycol (PEG). The binder and the plasticizer may be directly added and mixed with the slurry, or dissolved in a solvent in advance and then added to the slurry.
3. Pouring: porous alumina casting slurry with appropriate viscosity was cast on an aluminum nitride ceramic substrate with a doctor blade with adjustable gap. The thickness of the cast tape was adjusted by the doctor blade gap, slurry viscosity and casting rate. The cast tape is dried in an air or oxygen atmosphere with or without heating the substrate. After evaporation of the solvent and pore former from the casting belt, green sheets of different thicknesses were obtained. And continuously pouring the YAG casting slurry on the porous alumina green sheet by using a scraping blade with an adjustable gap to form a porous alumina and YAG green sheet layer stacked on the heat-conducting substrate.
4. Laminating: the stack of cast tapes is placed between metal molds made of metal such as stainless steel, heated to above the Tg temperature (glass transition temperature) of the adhesive, then uniaxially compacted, and then released from the pressure. In this process, a pattern such as holes, pillars, or a rough surface on a green sheet is formed on the green sheet by using a mold having a designed pattern in lamination. Such a pattern may improve light coupling and reduce lateral light propagation by waveguide effects, thereby facilitating light extraction in the light output direction.
5. And (3) sintering: the green sheet is heated in air to decompose organic components such as binders, plasticizers. After binder removal, the green sheet is placed under vacuum, H2/N2、H2And/or Ar/H2Sintering in an atmosphere at a temperature in the range of 1200 ℃ to 1900 ℃, preferably 1500 ℃ to 1800 ℃, more preferably 1600 ℃ to 1700 ℃ for 1 hour to 100 hours, preferably 2 to 10 hours. Binder removal and sintering processCan be carried out independently or together. Laminated green sheets sintered under a reducing atmosphere are generally brown or dark brown in color during sintering due to the formation of defects such as oxygen vacancies. It is generally necessary to carry out reoxidation in an air or oxygen atmosphere in order to obtain a ceramic sheet having a high luminous efficiency in the visible wavelength range.
Example two
The basic composition of the luminescent ceramic structure of this embodiment is the same as that of the first embodiment, and the only difference is that: the alumina porous ceramic is doped with magnesium oxide instead of zinc oxide.
EXAMPLE III
The basic composition of the luminescent ceramic structure of this embodiment is the same as that of the first embodiment, and the only difference is that: the alumina porous ceramic is doped with magnesium oxide and zinc oxide.
As analyzed, the present embodiment has ZnAl between the porous ceramic reflective layer 120 and the ceramic heat-dissipating substrate 1302O4And MgAl2O4And (4) generating.
Example four
The basic composition of the luminescent ceramic structure of this embodiment is the same as that of the first embodiment, and the only difference is that: in the porous ceramic reflective layer 120, zirconia and yttria are further doped in addition to zinc oxide and/or magnesium oxide.
EXAMPLE five
As shown in fig. 2, the basic composition of the luminescent ceramic structure of this embodiment is the same as that of the first embodiment, and the only difference is that: the luminescent ceramic layer 110 is coated with a plurality of alternating antireflection films 140 of high refractive index films and low refractive index films to further improve the blue light transmittance and the light extraction efficiency.
EXAMPLE six
As shown in fig. 3, the basic composition of the luminescent ceramic structure of this embodiment is the same as that of the first embodiment, and the only difference is that: the light-emitting ceramic layer 110 is etched to form a saw-tooth structure 150 for further improving the light-emitting efficiency.
The foregoing is a more detailed description of the present invention that is presented in conjunction with specific embodiments, and the practice of the invention is not to be considered limited to those descriptions. For those skilled in the art to which the invention pertains, several simple deductions or substitutions can be made without departing from the spirit of the invention, and all shall be considered as belonging to the protection scope of the invention.
Claims (9)
1. A luminescent ceramic structure is characterized by comprising a luminescent ceramic layer, a porous ceramic reflecting layer and a ceramic heat dissipation substrate which are sequentially laminated and combined together; wherein the porous ceramic reflective layer is an alumina porous ceramic doped with zinc oxide and/or magnesium oxide for bonding with the ceramic heat dissipation substrate; and at least part of the doped zinc oxide is ZnxAlyO, and at least part of the doped magnesium oxide is MgxAlyThe form of O exists; the ceramic heat dissipation substrate is an aluminum nitride ceramic substrate; the proportion of the doped oxide in the porous ceramic reflecting layer is 1-10% of the total mass.
2. The luminescent ceramic structure of claim 1, wherein the ZnxAlyO is in particular ZnAl2O4，MgxAlyO is in particular MgAl2O4。
3. The luminescent ceramic structure of claim 1, wherein the porous ceramic reflective layer is further doped with at least one of zirconia, titania, and yttria.
4. The luminescent ceramic structure of claim 1, wherein the luminescent ceramic layer is a Ce-doped YAG ceramic.
5. The luminescent ceramic structure according to any one of claims 1 to 4, wherein the luminescent ceramic layer has a thickness of 0.05 to 1mm, the porous ceramic reflective layer has a thickness of 0.1 to 2mm, and the ceramic heat dissipation substrate has a thickness of 0.5 to 5 mm.
6. The luminescent ceramic structure of claim 1, wherein the luminescent ceramic layer has an antireflection coating on its surface or a rough microstructure on its surface.
7. A method of making a luminescent ceramic structure according to any of claims 1 to 6, comprising: casting slurry respectively used for forming the porous ceramic reflecting layer and the luminescent ceramic layer is sequentially poured on the ceramic heat dissipation substrate, and then the luminescent ceramic structure is formed through lamination and sintering in sequence.
8. A light-emitting device comprising the luminescent ceramic structure according to any one of claims 1 to 6, and further comprising an excitation light source for generating excitation light, wherein the luminescent ceramic structure is located in an optical path of the excitation light.
9. A projection system comprising the light-emitting device of claim 8 and further comprising a projection imaging device.
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| PCT/CN2017/109330 WO2018095211A1 (en) | 2016-11-25 | 2017-11-03 | Luminescent ceramic structure and preparation method therefor, and related light-emitting device and projecting device |
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| CN111072374B (en) * | 2018-10-18 | 2022-05-06 | 深圳光峰科技股份有限公司 | Fluorescent ceramic and preparation method thereof |
| CN112939578B (en) * | 2019-11-26 | 2023-07-18 | 深圳市中光工业技术研究院 | Fluorescent ceramic, preparation method thereof, light-emitting device and projection device |
| CN111393151A (en) * | 2020-03-26 | 2020-07-10 | 郑州中瓷科技有限公司 | Zirconia-doped alumina ceramic substrate and preparation process thereof |
| CN111792947B (en) * | 2020-06-22 | 2022-07-22 | 佛山欧神诺陶瓷有限公司 | Foamed ceramic with fluorescent decorative effect and preparation method thereof |
| CN116867752A (en) * | 2020-12-18 | 2023-10-10 | 贺利氏科纳米北美有限责任公司 | Multilayer sintered ceramic body |
| CN112851124B (en) * | 2021-02-04 | 2022-03-22 | 中国科学院福建物质结构研究所 | Glass ceramic membrane composite material for laser illumination |
| CN118213453B (en) * | 2024-05-22 | 2024-08-13 | 华引芯（武汉）科技有限公司 | Fluorescent film, preparation method thereof and light-emitting element |
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