CN115895657A - Fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina and preparation method and application thereof - Google Patents

Fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina and preparation method and application thereof Download PDF

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CN115895657A
CN115895657A CN202211240768.7A CN202211240768A CN115895657A CN 115895657 A CN115895657 A CN 115895657A CN 202211240768 A CN202211240768 A CN 202211240768A CN 115895657 A CN115895657 A CN 115895657A
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metal aluminum
mesoporous alumina
emission layer
based mesoporous
alumina
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CN115895657B (en
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王乐
解荣军
周天亮
张宏
邾强强
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Xiamen University
China Jiliang University
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China Jiliang University
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Abstract

The invention provides a fluorescence emission layer prepared based on metal aluminum-based mesoporous alumina, and a preparation method and application of the fluorescence emission layer. The chemical general formula of the fluorescent emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1; under the excitation of blue light of 450nm, the wavelength range of an emission spectrum generated by the fluorescence emission layer is 460-760 nm, and the main peak of the emission spectrum is 530-550 nm. Compared with the prior art, the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina has a simple integral structure and is easy to synthesize; the fluorescence emission layer directly grows on the aluminum plate, and after the fluorescence emission layer is excited by laser, heat generated by the fluorescence emission layer is quickly conducted away without being conducted away by virtue of good heat conduction capability of the aluminum plateCan generate heat accumulation, can not cause obvious temperature rise of the fluorescent emission layer, and can be used for laser illumination.

Description

Fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina and preparation method and application thereof
Technical Field
The invention relates to the technical field of illumination, in particular to a fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina, and a preparation method and application thereof.
Background
With the continuous progress of industrial technology, the lighting technology is also continuously upgraded and updated. From the first relying on natural animal and plant materials to fossil fuels and then to point sources of light such as incandescent and fluorescent lamps. In the last 90 s, energy-saving and efficient white light LED solid-state lighting began to appear. And because the cost of the laser diode is gradually reduced, the performance tends to be stable, so that the adoption of laser as a lighting source becomes possible.
The laser lighting technology has the technical principle similar to that of the white light LED technology. In the white light LED lighting technology, a blue (or violet, etc.) LED chip excites a fluorescent material, and light emitted from the LED chip and light emitted from the fluorescent material after excitation are combined together to obtain white light. The laser illumination technology is generally implemented by using laser diodes (most commonly laser diodes capable of emitting blue light) to excite fluorescent materials, and combining light emitted by the laser diodes with light emitted by the excited fluorescent materials to finally obtain white light, as described in patent document 1 (Wang Dajian, song Weiwei, mao Zhiyong, li Anhao, sun Tao, lu Zhijuan, a remote fluorescent coating for high-efficiency laser illumination and application thereof, ZL 201410609545.2).
Laser illumination techniques face a number of unique technical challenges. Among them is the most troublesome: heating of the fluorescent material. This is because, due to internal defects, energy transfer, and the like, the light conversion efficiency (quantum efficiency) of the fluorescent material under blue laser light is generally less than 100%, and therefore a considerable portion of the laser energy is converted into heat, resulting in an increase in the temperature of the fluorescent material, which causes significant thermal quenching of the fluorescent material (resulting in a decrease in the emission intensity). In addition, for example, a common blue laser excites a yellow fluorescent material, and for the yellow fluorescent material, when the yellow fluorescent material absorbs blue light and converts the blue light into yellow light, due to the difference of wavelengths between the blue light and the yellow light, there is an energy difference, i.e., stokes shift, between the blue light and the yellow light. Therefore, regardless of the quantum efficiency of the phosphor, when the yellow phosphor is excited by the blue light, the energy loss is inevitable and cannot be eliminated. This energy loss must be converted to heat. The fluorescent material has thermal quenching characteristics, that is, as the temperature increases, the luminescent performance of the fluorescent material decreases. And because the laser is collimated light, the power density of the laser spot is extremely high because the light beam is concentrated. Therefore, when the laser irradiates the surface of the fluorescent material, the temperature of the fluorescent material is increased more obviously.
Therefore, the most important technical means for laser illumination is to remove (conduct) the heat generated by the fluorescent material under the laser irradiation. Common technical means include ceramming or vitrifying the phosphor material onto a highly thermally conductive substrate, or dispersing the phosphor material into a thermally conductive material. In fact, there is considerable literature in this area of technology. For example, patent document 2 (r.coulter, r.r.dergenten, e.j.m.paupe Lu Sen, a.walster, D. Funier, lamp for laser application, CN 102482576B) discloses a method to solve the problem of heat generation and reduce heat accumulation in the phosphor. The optical performance for laser applications is improved while heat transfer is promoted by the transparent body containing the phosphor. This method, in particular the attachment between the holder and the phosphor, is preferably achieved by means of a molten glass, a ceramic glue, more preferably by means of a transparent pressure ceramic or silicon thermal interface material. However, overall, there are many interfaces between devices, the thermal resistance is high, and the heat conductivity of the devices is general, and the heat generated after the laser irradiates the fluorescent material cannot be quickly conducted away.
Patent document 3 (Wang Dajian, gao Wenyu, mao Zhiyong, chen Jingjing, tian Hua, yang Chao, ann, shi Yuandong, low-melting glass frit and glass ceramic for laser illumination produced therefrom, CN 106587641B) discloses a low-melting glass frit and glass ceramic for laser illumination produced therefrom. The low-melting-point glass powder has lower glass phase transition temperature, the glass phase transition temperature of the low-melting-point glass powder can be adjusted within the range of 200-500 ℃, and the low-melting-point glass powder is suitable for manufacturing sealing glass and vacuum components and packaging LEDs (light emitting diodes), is particularly suitable for manufacturing luminescent glass ceramics with fluorescent powder materials, and is particularly suitable for laser illumination. The glass ceramic is molded and sintered at a lower temperature, so that the thermal degradation of the fluorescent powder at a high temperature can be effectively avoided, and the glass ceramic has an important application value in the field of laser illumination. However, in general, the thermal conductivity of glass is relatively low, and heat generated after laser light irradiates the fluorescent material cannot be rapidly conducted away.
Patent document 4 (Feng Shaowei, xia Xiaochun, royal red, zhu Jinchao, li Chunhui, zhang Pande, she Yong, li Dongsheng, full spectrum multiphase fluorescent ceramic for laser illumination and display and preparation method, CN 111285682A) discloses a full spectrum multiphase fluorescent ceramic for laser illumination and laser display, and the invention has the beneficial effects that: the light-emitting material has a completely compact microstructure, excellent thermal conductivity and mechanical properties, can effectively improve the heat generated by the light-emitting material, reduces the overall temperature of the device, and improves the light extraction efficiency. However, in general, compared with glass, the thermal conductivity of the fluorescent ceramic is significantly improved, but the preparation process of the fluorescent ceramic is too complex.
Patent document 5 (Li Qian, xu Yanzheng, wavelength conversion device and its light source system, projection system, CN 203489180U) discloses a wavelength conversion device and its light source system, projection system. The wavelength conversion device comprises a support and a plurality of wavelength conversion modules spliced with each other, wherein each wavelength conversion module comprises a ceramic carrier and fluorescent powder arranged on the ceramic carrier, and the support keeps the plurality of wavelength conversion modules relatively fixed. The light source system and the projection system both comprise the wavelength conversion device. Adopt the utility model discloses, utilize ceramic material as the ceramic carrier of phosphor powder, can be high temperature resistant, and can not lead to the phosphor powder to be difficult to adhere to because of high temperature warp. Obviously, ceramization of fluorescent materials is a common method in the art for conducting heat away and reducing the temperature of devices. Since the fluorescent ceramic itself is light transmissive, the most suitable device structure is obviously transmissive, i.e., the excitation light passes through the fluorescent ceramic itself.
The ceramming process is also used, but the thermal conductivity of the device can also be improved by creating a second phase. Patent document 6 (Zhu Ning, multiphase fluorescent ceramic for blue light excited white light illumination, preparation method and light source device, CN 109896852A) discloses multiphase fluorescent ceramic for blue light excited white light illumination, preparation method and light source device. The complex phase fluorescent ceramic has fluorescent phase with lutetium aluminum garnet structure and Al 2 O 3 A high thermal conductivity phase of said Al 2 O 3 The microcrystals in the high thermal conductivity phase are uniformly distributed and surround the lutetium aluminum garnet fluorescent phase, and form a three-dimensional network channel to reach the surface of the complex phase fluorescent ceramic. The invention has the beneficial effects that: the problems that the thermal shock resistance of the fluorescent material is weak, the luminous efficiency of the fluorescent material is reduced along with the increase of the temperature and the like in the conventional white light laser illumination are effectively solved. However, overall, due to the introduction of the second phase, although the heat conduction effect of the material is obviously improved, the luminous efficiency of the obtained material is lower than that of the conventional fluorescent ceramic.
Besides the ceramic process, the fluorescent material is combined with the thin-film process of the low-melting-point glass powder, and the heat generated by the fluorescent material under the excitation of laser can be well conducted away. For example, patent document 7 (jirong army, shanghai, zheng Peng, zhou Tianliang, li Shuxing, nitride phosphor/glass composite light conversion member for laser illumination and preparation thereof, CN 108895314B) discloses a nitride phosphor/glass composite light conversion member for laser illumination. The nitride fluorescent powder/glass composite coating is composed of a nitride fluorescent powder/glass composite coating and a high-thermal-conductivity ceramic matrix, wherein the nitride fluorescent powder/glass composite coating is tightly grown on the high-thermal-conductivity ceramic matrix. However, overall, although the ceramic thermal conductivity coefficient as the substrate is high, an obvious interface exists at the joint of the phosphor/glass composite coating and the ceramic substrate, the thermal resistance is high, and the thermal conduction effect of the obtained phosphor/glass composite light conversion component needs to be improved.
In addition, it is also important to consider the heat generated by both the laser diode and the fluorescent material to perform necessary thermal management. For example, patent document 8 (Cao Yongge, xia Zejiang, shen Xiaofei, maokang, laser white light emitting device for illumination or display, CN 105826457B) discloses a laser white light emitting device for illumination or display. The invention combines the transparent fluorescent ceramic with the chip of the excitation light source, thereby avoiding the reduction of the luminous efficiency or the failure of the light source caused by the heating of the fluorescent powder and the silica gel; if the heat resistance of the transparent fluorescent ceramic is required according to application, the device can work in a high-current high-temperature environment, and the reduction of the output power and the electro-optic conversion efficiency of a device in high-temperature or high-injection current work is avoided. But overall, the device fabrication process is too complex.
Non-patent document 1 (Camman Yan, xinrui Ding, mingqi Chen, yifu Liang, shu Yang, yong Tang, research on Laser Illumination Based on Phosphor In Metal (PiM) by Y Ultilizing the Boron Nitride-Coated coater Foams, ACS applied. Mater. Interfaces 2021,13,25,29996-30007) reports a Laser illuminator device. The device is a metal Phosphor (PiM) converter formed by embedding a mixture of yellow phosphor and silica gel in BN/copper foam. The foam copper is used as a heat transfer channel communicated with the inside; the BN coating effectively solves the light absorption problem of the foam copper. It should be noted that although this solution can conduct away the heat generated by the fluorescent material to a certain extent through the copper foam, the problem of heat conduction of the fluorescent material under the laser illumination condition cannot be solved well due to the non-tight connection between the fluorescent material and the copper foam (the fluorescent material is fixed to the copper foam by using the silica gel with a low thermal conductivity coefficient).
Of course, an improvement is easily conceivable based on non-patent document 1. Namely, the low-melting-point glass powder is used for replacing silica gel, then the foam copper is integrally heated, so that the glass powder is converted into glass liquid, and after cooling, the fluorescent material is fixed in the foam copper by the glass liquid. However, this solution also has certain disadvantages. This is because the glass obviously cannot form a chemical bond with the foam copper, and although the heat conduction effect of the glass is improved compared with the scheme that the silica gel is combined with the fluorescent material and placed in the foam copper, the improvement effect is not very significant.
Mesoporous alumina is a widely used support material. As described in patent document 9 (Pan Dahai, li Ruifeng, wang Xu, guo Min, shang, he Min, ma Jinggong, a highly thermally stable ordered mesoporous alumina material and a method for preparing the same, CN 103539173B), the mesoporous alumina material has advantages of good mechanical strength, high chemical stability, suitable isoelectric point, adjustable surface acid/alkalinity, and various different crystal phase structures, etc., and becomes the most widely used catalyst or catalyst carrier in chemical and petroleum industries, and plays an important role in reaction processes such as petroleum component cracking, hydrofining, hydrodesulfurization, hydrocarbon reforming hydrogen production, gas-phase oil component purification, automobile exhaust purification, etc.
However, as disclosed in patent document 10 (Lu Yong, wang Chunzheng, han Lupeng, zhao Anqi, liu, an aluminum matrix-mesoporous alumina composite material and a preparation method and application thereof, CN 104148040B), compared with the conventional mesoporous alumina, the metal aluminum matrix mesoporous alumina has the advantages of good thermal conductivity, high permeability, easy molding, easy filling, easy storage and the like, and is an ideal catalyst carrier, and can be used as a catalyst carrier for preparing a catalyst for loading an active metal or loading an active metal and an auxiliary metal oxide. Obviously, the aluminum matrix-mesoporous alumina composite is also a recognized catalyst support material, as well as mesoporous alumina.
In summary, it can be seen from the prior publications that the metal aluminum based mesoporous alumina is not a material that is easily conceivable in the route of the laser illumination technology, and is difficult to apply to the laser illumination technology.
Disclosure of Invention
The invention aims to provide a fluorescent emitting layer prepared on the basis of metal aluminum-based mesoporous alumina.
The metal aluminum-based mesoporous alumina is a metal aluminum plate of which one side contains mesoporous alumina with the aperture size of 2-50 nm and the thickness of 20-200 mu m; the chemical formula of the fluorescent emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1. Under the excitation of blue light of 450nm, the metal aluminum base mesoporous is oxidizedThe wavelength range of an emission spectrum generated by the fluorescent emission layer prepared from aluminum is 460-760 nm, and the main peak of the emission spectrum is 530-550 nm; preferably, in the chemical formula of the fluorescent emission layer, a =4.5 and b =0.04.
The second purpose of the invention is to provide a preparation method of a fluorescence emission layer prepared based on metal aluminum-based mesoporous alumina. The preparation method comprises the following steps: 1) Preparing a Y precursor and a Ce precursor into an aqueous solution with the mass concentration of 50%; the molar ratio of Y to Ce in the Y precursor and Ce precursor is 2: b, wherein the molar ratio is 0.01<b<0.1; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 24-48 h; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 24-48 h under the condition of hydrogen or nitrogen-hydrogen mixed gas atmosphere and the temperature of 600-625 ℃ to obtain the metal aluminum-based mesoporous alumina prepared based on the metal aluminum-based mesoporous alumina and having the chemical general formula of Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is not less than 3 and not more than 6,0.01<b<0.1. Preferably, the volume content of hydrogen in the nitrogen-hydrogen mixed gas is 10-25%.
The invention also provides a laser lighting device with a reflection type structure, which comprises a blue laser diode and a fluorescence emission layer which is arranged opposite to the blue laser diode and is prepared on the basis of metal aluminum-based mesoporous alumina.
The specific scheme is as follows:
a fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina has a chemical general formula of Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1; further, in the chemical formula of the fluorescent emission layer, a =4.5 and b =0.04. The fluorescence emission layer is prepared on the basis of metal aluminum-based mesoporous alumina, and the metal aluminum-based mesoporous alumina is a metal aluminum plate with a single surface containing mesoporous alumina; the pore size of the mesoporous alumina is 2-50 nm, and the thickness is 20-200 μm.
Further, under the excitation of blue light of 450nm, the wavelength range of an emission spectrum generated by the fluorescence emission layer is 460-760 nm, and the main peak of the emission spectrum is 530-550 nm.
The invention also provides a preparation method of the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina, which comprises the following steps: 1) Preparing a Y precursor and a Ce precursor into an aqueous solution with the mass concentration of 40-60% (more preferably 50%); 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for a certain time; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and putting the solution into a vacuum oven for drying; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and carrying out high-temperature reaction in a reducing atmosphere to obtain a fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina, wherein the chemical general formula of the fluorescence emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1。
Further, the Y precursor is selected from nitrate of Y;
optionally, the Ce precursor is selected from the nitrate of Ce;
optionally, the purity of the Y precursor and the Ce precursor is not lower than 99.5wt%.
Further, the molar ratio of Y to Ce in the Y precursor and the Ce precursor is 2: b, wherein 0.01-b-0.1.
Optionally, the metal aluminum-based mesoporous alumina is a metal aluminum plate with a single surface containing mesoporous alumina; the pore size of the mesoporous alumina is 2-50 nm; the thickness of the mesoporous alumina is 20-200 μm;
optionally, the soaking time is 24-48 h;
optionally, drying at 70-90 deg.C for 18-30 h, more preferably, vacuum drying at 80 deg.C for 24h.
Further, the temperature of the high-temperature solid-phase reaction is 600-625 ℃, and the time of the high-temperature reaction is 24-48 h;
optionally, the reducing atmosphere is hydrogen or a nitrogen-hydrogen mixed gas; preferably, the volume content of hydrogen in the nitrogen-hydrogen mixed gas is 10-25%.
The invention also provides a laser lighting device which comprises a blue laser diode and a fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The laser lighting device is of a reflection type structure, and a light outlet of the blue laser diode is opposite to the fluorescence emission layer.
Compared with the prior art, the invention has the following beneficial effects:
the invention provides a fluorescence emission layer prepared based on metal aluminum-based mesoporous alumina, and a preparation method and application of the fluorescence emission layer. The chemical formula of the fluorescent emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1; under the excitation of blue light of 450nm, the wavelength range of an emission spectrum generated by the fluorescence emission layer is 460-760 nm, and the main peak of the emission spectrum is 530-550 nm. Compared with the prior art, the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina has a simple integral structure and is easy to synthesize; the fluorescence emission layer directly grows on the aluminum plate, and after the fluorescence emission layer is excited by laser, heat generated by the fluorescence emission layer is quickly conducted away by means of good heat conduction capability of the aluminum plate, so that heat accumulation can not be generated, the fluorescence emission layer can not generate obvious temperature rise, and the fluorescence emission layer can be used for laser illumination.
Drawings
FIG. 1 is an emission spectrum of a fluorescent light-emitting layer obtained in comparative example 1 of the present invention;
FIG. 2 is an emission spectrum of the fluorescent emitting layer obtained in comparative example 2 of the present invention;
FIG. 3 is a graph showing an emission spectrum of a fluorescent light-emitting layer obtained in example 1 of the present invention;
fig. 4 is a graph showing an emission spectrum of the laser-illuminated device obtained in example 17 of the present invention;
FIG. 5 is a structural view of a laser lighting device obtained in example 17 of the present invention
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention.
For the purpose of facilitating an understanding of the present invention, the present invention will now be described by way of examples. It should be understood by those skilled in the art that the examples are only for the purpose of facilitating understanding of the present invention and should not be construed as specifically limiting the present invention.
It should be noted that the embodiments and features of the embodiments in the present application may be combined with each other without conflict. The present invention will be described in detail with reference to examples.
The chemical general formula of the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina is as follows:
Y 2 O 3 ·aAl 2 O 3 ·bCeO 2
wherein a is more than or equal to 3 and less than or equal to 6, and the cover (b) is more than or equal to 0.01 and is covered with 0.1. In some embodiments provided herein, a is preferably 3,b is preferably 0.015; in some embodiments provided herein, a is preferably 3,b is preferably 0.02; in some embodiments provided herein, a is preferably 3,b is preferably 0.04; in some embodiments provided herein, a is preferably 3,b is preferably 0.08; in some embodiments provided herein, a is preferably 3,b is preferably 0.09; in some embodiments provided herein, a is preferably 3,b is preferably 0.095; in some embodiments provided herein, a is preferably 3.5, b is preferably 0.04; in some embodiments provided herein, a is preferably 4,b is preferably 0.04; in some embodiments provided herein, a is preferably 4.5, b is preferably 0.04; in some embodiments provided herein, a is preferably 5,b is preferably 0.04; in some embodiments provided herein, a is preferably 5.5, b is preferably 0.04; in some embodiments provided herein, a is preferably 5.9, b is preferably 0.04; in some embodiments provided herein, a is preferably 6,b is preferably 0.04; in some embodiments provided herein, a is preferably 4.5, b is preferably 0.02; in some embodiments provided herein, a is preferably 4.5, b is preferably 0.03; in other embodiments of the present invention, a is preferably 4.5, and b is preferably 0.05.
The preparation method of the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina comprises the following specific steps:
1) Preparing a Y precursor and a Ce precursor into an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for a certain time; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and putting the solution into a vacuum oven for drying; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and carrying out high-temperature reaction in a reducing atmosphere to obtain a fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina, wherein the chemical general formula of the fluorescence emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1。
In the step, the precursor of Y is selected from nitrate of Y; the Ce precursor is selected from the nitrate of Ce. The molar ratio of Y to Ce in the Y precursor and the Ce precursor is 2: b, wherein 0.01-b-0.1.
The purity of the Y precursor and the purity of the Ce precursor are both not lower than 99.5%, and the higher the purity is, the less impurities are in the obtained luminescent material.
The metal aluminum-based mesoporous alumina is a metal aluminum plate with a single surface containing mesoporous alumina. The pore size of the metal aluminum-based mesoporous alumina is 2-50 nm, and the thickness of the mesoporous alumina is preferably 20-200 μm. In some embodiments provided herein, the mesoporous alumina preferably has a pore size of 3nm and a thickness of 25 μm; in some embodiments provided herein, the mesoporous alumina preferably has a pore size of 20nm and a thickness of 100 μm; in some embodiments provided herein, the mesoporous alumina preferably has a pore size of 45nm and a thickness of 150 μm; in other embodiments provided herein, the mesoporous alumina preferably has a pore size of 40nm and a thickness of 180 μm.
The soaking time is 24-48 h, and in some embodiments provided by the invention, the soaking time is preferably 36h.
The temperature of the vacuum drying is 80 ℃, and the drying time is 24h.
In the step, the reducing atmosphere is hydrogen or nitrogen-hydrogen mixed gas, preferably, the volume content of hydrogen in the nitrogen-hydrogen mixed gas is 10-25%; in the present invention, a nitrogen-hydrogen mixed gas is preferred.
The temperature of the high-temperature solid phase in the step is preferably 600-625 ℃, the atmosphere is nitrogen-hydrogen mixed gas, and in some embodiments provided by the invention, the temperature of the high-temperature solid phase is preferably 600 ℃; in other embodiments provided herein, the temperature of the high temperature solid phase is preferably 625 ℃.
The time of the high-temperature solid phase in the step is preferably 24 to 48 hours, and more preferably 36 to 48 hours; in some embodiments provided herein, the time of the high temperature solid phase is preferably 36 hours.
The high temperature solid reaction phase is preferably carried out in a high temperature furnace. After the reaction is carried out, the reaction product is cooled to room temperature along with the furnace, and the fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina can be obtained.
The invention adopts high-temperature solid-phase reaction to successfully prepare the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina.
The laser lighting device with the reflection type structure at least comprises a blue laser diode and a fluorescence emission layer prepared on the basis of metal aluminum-based mesoporous alumina. The chemical general formula of the fluorescence emission layer prepared based on the metal aluminum-based mesoporous alumina is as follows: y is 2 O 3 ·aAl 2 O 3 ·bCeO 2 (wherein, a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1)。
In order to further illustrate the present invention, the following describes in detail a fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina, and a preparation method and a device thereof, which are provided by the present invention, with reference to examples.
The reagents used in the following comparative examples and examples are all commercially available.
In the mixed atmosphere of nitrogen and hydrogen used in the following comparative examples and examples, the hydrogen content was 20% by volume.
The Y precursor and the Ce precursor used in the comparative example and the example are only examples and do not limit the raw materials of the precursors, and the purity of the precursors is not lower than 99.5wt%.
Comparative example 1
The chemical formula of the material of this comparative example is: y is 2 O 3 ·1.667Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 40nm and the thickness of the mesoporous alumina of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·1.667Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·1.667Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the resulting fluorescent emission layer was measured using a fluorescence spectrometer, and it was found that the resulting fluorescent emission layer emitted light weakly and hardly (see fig. 1).
Comparative example 2
The chemical formula of the material described in this comparative example is: y is 2 O 3 ·2Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 40nm and the thickness of mesoporous alumina of 180 mu m according to the size and the thickness of mesopores and metal aluminumThe external dimension of the base mesoporous alumina is calculated by firstly calculating the mole number of alumina in the metal aluminum base mesoporous alumina and then adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·2Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain the metal aluminum-based mesoporous alumina with the chemical general formula of Y 2 O 3 ·2Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the resulting fluorescent emission layer was measured using a fluorescence spectrometer, and the resulting fluorescent emission layer was found to emit extremely weak light with little emission (see fig. 2).
Comparative example 3
The chemical formula of the material of this comparative example is: y is 2 O 3 ·2.9Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 40nm and the thickness of the mesoporous alumina of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·2.9Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 DEG CDrying for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·2.9Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer is very weak in luminescence.
Comparative example 4
The chemical formula of the material described in this comparative example is: y is 2 O 3 ·6.5Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 40nm and the thickness of mesoporous alumina of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then using Y (NO) to obtain the product 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·6.5Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·6.5Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer is very weak in light emission.
Comparative example 5
Conversion of the materials described in this comparative exampleThe chemical formula is: y is 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 . Selecting single-sided metal aluminum-based macroporous alumina with the pore size of 70nm and the thickness of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based macroporous alumina according to the pore size and the thickness of the macroporous alumina and the external dimension of the metal aluminum-based macroporous alumina, and then using Y (NO) as the raw material 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based macroporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based macroporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based macroporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based macroporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain the metal aluminum-based macroporous alumina with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 And a fluorescence emission layer prepared based on the metal aluminum-based macroporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer is very weak in light emission.
Comparative example 6
The chemical formula of the material described in this comparative example is: y is 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 . Selecting single-sided metal aluminum-based microporous alumina with the aperture size of 1.8nm and the thickness of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based microporous alumina according to the aperture size and the thickness of the microporous alumina and the external dimension of the metal aluminum-based microporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting metal aluminum-based microporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based microporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based microporous alumina at 80 ℃ for 24 hours in vacuum; 4) Putting the metal aluminum-based microporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a metal aluminum-based microporous alumina with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based microporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer is very weak in luminescence.
Comparative example 7
In this comparative example, Y was selected as the chemical component 3 Al 5 O 12 0.06Ce, 300 μm thick ceramic plate, which was fixed to an aluminum plate with a heat conductive silica gel having a thermal conductivity of 1.5W/(m.K), 100 μm thick. After the heat-conducting silica gel is solidified, the power density is 5W/mm 2 The ceramic wafer was irradiated with the 450nm blue laser, and after 10 minutes, the temperature rise of the ceramic wafer was high (see table 1). Obviously, the ceramic plate generates obvious temperature rise after being irradiated by laser because of the obvious interface layer between the ceramic plate and the aluminum plate and the larger thermal resistance, and the temperature rise inevitably causes the fluorescent material to generate obvious thermal quenching.
Example 1
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the pore size of 3nm and the thickness of mesoporous alumina of 25 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then using Y (NO) to obtain the product 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 Chemical meterAccurately weighing the raw materials according to the weight ratio, and then 1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 600 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.015CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer was measured using a fluorescence spectrometer, and it was found that the obtained fluorescence emission layer emitted light strongly, the wavelength range of the emission spectrum was 460 to 760nm, and the main peak of the emission spectrum was 531nm (see fig. 3). Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 2
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.02CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 20nm and the thickness of the mesoporous alumina of 100 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.02CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and carrying out nitrogen and hydrogenReacting for 36 hours under the condition of mixed gas atmosphere and temperature of 625 ℃ to obtain a chemical general formula Y 2 O 3 ·3Al 2 O 3 ·0.02CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 3
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 Irradiating the fluorescent emission layer with 450nm blue laser for 10 minThen, the temperature rise of the fluorescence emitting layer was low (see table 1).
Example 4
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.08CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 40nm and the thickness of the mesoporous alumina of 180 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.08CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.08CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer has strong luminescence. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 5
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.09CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of 150 mu m of mesoporous alumina, and firstly calculating the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous aluminaThe number of moles of alumina in the aluminum, then Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.09CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.09CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer has strong luminescence. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 6
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·3Al 2 O 3 ·0.095CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3Al 2 O 3 ·0.095CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Step 2) Taking out the soaked metal aluminum-based mesoporous alumina from the solution, and vacuum-drying at 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain the metal aluminum-based mesoporous alumina with the chemical general formula of Y 2 O 3 ·3Al 2 O 3 ·0.095CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. The power density of the power is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 7
The chemical formula of the material in this example is: y is 2 O 3 ·3.5Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·3.5Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 600 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·3.5Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. Measuring the resulting fluorescent emission layer using a fluorescence spectrometerThe emission spectrum, the position of the main peak of the emission spectrum and the intensity are shown in table 1, and the obtained fluorescent emission layer has strong luminescence. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 8
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·4Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·4Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·4Al 2 O 3 ·0.04CeO 2 And a fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 9
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·4.5Al 2 O 3 ·0.04CeO 2 . Selecting a pore size of45nm of single-sided metal aluminum-based mesoporous alumina with the thickness of 150 mu m, calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the reference 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. The power density of the power is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 10
The chemical formula of the material in this example is: y is 2 O 3 ·5Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then using Y (NO) to obtain the mesoporous alumina 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·5Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·5Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 After irradiating the fluorescent emission layer with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emission layer was low (see table 1).
Example 11
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·5.5Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·5.5Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a chemical general formulaIs Y 2 O 3 ·5.5Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 12
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·5.9Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·5.9Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·5.9Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. The power density of the power is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 13
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·6Al 2 O 3 ·0.04CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then using Y (NO) to obtain the mesoporous alumina 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·6Al 2 O 3 ·0.04CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain the metal aluminum-based mesoporous alumina with the chemical general formula of Y 2 O 3 ·6Al 2 O 3 ·0.04CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. The power density of the power is 5W/mm 2 After irradiating the fluorescent emission layer with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emission layer was low (see table 1).
Example 14
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·4.5Al 2 O 3 ·0.02CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.02CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.02CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer has strong luminescence. Using power the density is 5W/mm 2 After irradiating the fluorescent emission layer with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emission layer was low (see table 1).
Example 15
The chemical formula of the material in the embodiment is as follows: y is 2 O 3 ·4.5Al 2 O 3 ·0.03CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.03CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking the metal aluminum-based mesoporous alumina soaked in the step 2) out of the solutionTaking out, and vacuum drying for 24h at 80 ℃; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.03CeO 2 And a fluorescent emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in table 1, and the obtained fluorescence emission layer can be found to emit light strongly. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
Example 16
The chemical formula of the material in this example is: y is 2 O 3 ·4.5Al 2 O 3 ·0.05CeO 2 . Selecting single-sided metal aluminum-based mesoporous alumina with the aperture size of 45nm and the thickness of the mesoporous alumina of 150 mu m, firstly calculating the mole number of alumina in the metal aluminum-based mesoporous alumina according to the size and the thickness of mesopores and the external dimension of the metal aluminum-based mesoporous alumina, and then taking Y (NO) as the basis 3 ) 3 And Ce (NO) 3 ) 3 Is taken as a raw material and has a chemical formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.05CeO 2 Accurately weighing the raw materials in the stoichiometric ratio of (1) adding Y (NO) 3 ) 3 And Ce (NO) 3 ) 3 Preparing an aqueous solution with the mass concentration of 50%; 2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 36 hours; 3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, and drying the metal aluminum-based mesoporous alumina in vacuum at the temperature of 80 ℃ for 24 hours; 4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and reacting for 36 hours under the atmosphere of nitrogen and hydrogen mixed gas at the temperature of 625 ℃ to obtain a compound with the chemical general formula of Y 2 O 3 ·4.5Al 2 O 3 ·0.05CeO 2 And a fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina. The emission spectrum of the obtained fluorescence emission layer is measured by using a fluorescence spectrometer, the position and the intensity of the main peak of the emission spectrum are shown in a table 1,the resulting fluorescent emission layer was found to emit light strongly. Using power the density is 5W/mm 2 After the fluorescent emitting layer was irradiated with the 450nm blue laser for 10 minutes, the temperature rise of the fluorescent emitting layer was low (see table 1).
TABLE 1 emission spectra data sheet of materials
Figure BDA0003884664280000221
Example 17
The chemical component obtained in example 9 was Y 2 O 3 ·4.5Al 2 O 3 ·0.04CeO 2 The fluorescent emission layer prepared based on the metal aluminum-based mesoporous alumina is packaged with a blue laser diode with the emission wavelength of 450nm, and the fluorescent emission layer and the blue laser diode are oppositely arranged. Fig. 4 shows an emission spectrum of a laser lighting device obtained in example 17. Fig. 5 is a view showing a structure of a laser lighting device obtained in example 17.
001: a 450nm blue laser; 002: light incident to the fluorescent emission layer; 003: a fluorescent emission layer prepared based on metal aluminum-based mesoporous alumina; 004: a metal aluminum plate; 005: the 450nm blue light and the light emitted by the fluorescence emission layer under the excitation of the 450nm blue light are mixed.
The preferred embodiments of the present invention have been described in detail, however, the present invention is not limited to the specific details of the above embodiments, and various simple modifications may be made to the technical solution of the present invention within the technical idea of the present invention, and these simple modifications are within the protective scope of the present invention.
It should be noted that the various features described in the foregoing embodiments may be combined in any suitable manner without contradiction. The invention is not described in detail in order to avoid unnecessary repetition.
In addition, any combination of the various embodiments of the present invention can be made, and the same should be considered as the disclosure of the present invention as long as the idea of the present invention is not violated.

Claims (8)

1. A fluorescence emission layer prepared based on metal aluminum-based mesoporous alumina is characterized by comprising: the fluorescent material comprises metal aluminum-based mesoporous alumina and a fluorescent emission layer arranged on the metal aluminum-based mesoporous alumina;
the metal aluminum-based mesoporous alumina is a metal aluminum plate with a single surface containing mesoporous alumina, the pore size of the mesoporous alumina is 2-50 nm, and the thickness of the mesoporous alumina is 20-200 mu m;
the chemical general formula of the fluorescence emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1。
2. The fluorescence emission layer prepared based on metal aluminum-based mesoporous alumina according to claim 1, wherein in the chemical formula of the fluorescence emission layer, a =4.5, b =0.04.
3. The fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina as claimed in claim 1 or 2, wherein the wavelength range of an emission spectrum generated by the fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina is 460-760 nm and the main peak of the emission spectrum is 530-550 nm under the excitation of blue light of 450 nm.
4. The method for preparing a fluorescence emitting layer prepared based on metal aluminum based mesoporous alumina according to any one of claims 1 to 3, comprising the following steps:
1) Preparing a Y precursor and a Ce precursor into an aqueous solution with the mass concentration of 40-60%, wherein the molar ratio of Y to Ce in the Y precursor and the Ce precursor is 2: b, and 0.01-straw-b-0.1;
2) Putting the metal aluminum-based mesoporous alumina into the solution obtained in the step 1), and soaking for 24-48 h;
3) Taking out the metal aluminum-based mesoporous alumina soaked in the step 2) from the solution, putting the solution into a vacuum oven, and drying the solution at the temperature of between 70 and 90 ℃ for 18 to 30 hours;
4) Putting the metal aluminum-based mesoporous alumina dried in the step 3) into a high-temperature furnace, and carrying out high-temperature reaction in a reducing atmosphere to obtain a fluorescence emission layer prepared on the basis of the metal aluminum-based mesoporous alumina, wherein the chemical general formula of the fluorescence emission layer is Y 2 O 3 ·aAl 2 O 3 ·bCeO 2 Wherein a is more than or equal to 3 and less than or equal to 6,0.01<b<0.1。
5. The method for preparing a fluorescent emitting layer based on metal aluminum-based mesoporous alumina as claimed in claim 4, wherein the Y precursor is selected from the group consisting of nitrate of Y; the Ce precursor is selected from nitrate of Ce, and the purity of the Y precursor and the purity of the Ce precursor are not lower than 99.5wt%.
6. The preparation method of the fluorescence emission layer prepared based on the metal aluminum based mesoporous alumina as claimed in claim 4 or 5, wherein the temperature of the high-temperature reaction is 600-625 ℃, and the time of the high-temperature reaction is 24-48 h; the reducing atmosphere is hydrogen or a nitrogen-hydrogen mixed gas.
7. A laser illumination device comprising a blue laser diode and a fluorescence emitting layer made of metal aluminum based mesoporous alumina according to claim 1.
8. The laser lighting device according to claim 7, wherein the laser lighting device is a reflective structure, and the light outlet of the blue laser diode is arranged opposite to a fluorescence emission layer made of metal aluminum-based mesoporous alumina.
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