CN115215646A - High-thermal-conductivity and high-thermal-stability three-phase fluorescent ceramic for laser illumination and preparation method thereof - Google Patents
High-thermal-conductivity and high-thermal-stability three-phase fluorescent ceramic for laser illumination and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a high-thermal-conductivity high-thermal-stability three-phase fluorescent ceramic for laser illumination and a preparation method thereof. The three-phase fluorescent ceramic is Ce: luAG-MgAl 2 O 4 MgO, ce: luAG as ceramic host, mgAl 2 O 4 MgO and MgO are high heat-conducting phases, and emit high-brightness broadband yellow light near 550nm under the excitation of a blue light LD chip with the wavelength near 455nm, and the heat conductivity is 28Wm ‑1 K ‑1 ～32Wm ‑1 K ‑1 The emission intensity only loses 1.4% -3.4% at 150 ℃, the emission intensity only loses 3.2% -5.8% at 250 ℃, and the high-heat-conductivity and high-heat-stability ceramic material has the advantages of high heat conductivity, short time, simple preparation method and sinteringThe temperature is low, and the LED/LDs device can be applied to high-power LED/LDs devices.
Description
Technical Field
The invention relates to the technical field of fluorescent ceramics, in particular to a high-thermal-conductivity and high-thermal-stability three-phase fluorescent ceramic for laser illumination and a preparation method thereof.
Background
The method of producing white light is to combine a blue light emitting diode with a yellow fluorescent conversion material (YAG: ce). Due to the high power laser irradiation, the phosphor conversion material must have good thermal properties in order to obtain good heat dissipation effect, and thus the garnet-based composite ceramic phosphor has received a lot of attention. By adding highly heat-conductive phases, e.g. Al 2 O 3 (32-35W m -1 K -1 )、MgAl 2 O 4 (22W m -1 K -1 )，MgO(47.2W m -1 K -1 -53.5W m -1 K -1 ) In addition to their thermal properties, the complex phase can also act as a scattering center by changing the direction of light propagation in the ceramic, thereby increasing the absorption of light. The complex phase having a lower refractive index than the main phase can also improve light extraction efficiency by reducing reflection loss of emitted light. Lu (light emitting diode) 3 Al 5 O 12 :Ce 3+ The (LuAG: ce) is obviously better than other fluorescence conversion materials in the aspect of thermal quenching, and the ceramic has good heat-conducting property, so the ceramic is very suitable for being used as the fluorescent conversion materialLaser illumination and display of the host material.
In the aspect of preparing complex phase ceramics by adopting LuAG as a matrix material, CN109896852A discloses complex phase fluorescent ceramics for blue light-excited white light illumination, a preparation method and a light source device 2 O 3 The preparation method has the disadvantages of long time, more preparation steps and relatively high sintering temperature, and limits the application of the preparation method in high-power LED/LDs devices.
Disclosure of Invention
The invention aims to provide a preparation method of a high-thermal-conductivity high-thermal-stability three-phase fluorescent ceramic for laser illumination, which has the advantages of simple steps, low sintering temperature and short time.
The invention also aims to provide the high-thermal-conductivity high-thermal-stability three-phase fluorescent ceramic for laser lighting prepared by the preparation method.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
in a first aspect, the invention provides a preparation method of a three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination, which comprises the following steps:
(1) Respectively weighing Ce, luAG powder and MgO powder according to the mass ratio to serve as ceramic raw material powder, wherein MgO accounts for 20% -50% of the total mass of the ceramic raw material powder;
(2) Blending Ce, luAG and MgO, adding absolute ethyl alcohol, and fully mixing by ball milling;
(3) Taking out and drying the slurry obtained after ball milling to obtain dry powder;
(4) And wrapping the dried powder with graphite paper, performing discharge plasma sintering in a vacuum state, and cooling to room temperature to obtain the three-phase fluorescent ceramic.
Preferably, in the step (1), the particle size of the Ce: luAG powder is 1-1.3 μm, the particle size of the MgO powder is 1.5-2 μm, and the purity is more than 99.99%.
Preferably, the sintering pressure of the spark plasma sintering in the step (4) is 50-100 MPa, the pulse current is 200-400A, the heat preservation sintering time is 20-50 min, and the sintering temperature is 1480-1600 ℃.
Preferably, the ball milling rotation speed in the step (2) is 180-250 rpm, and the ball milling time is 15-30 h.
Preferably, the drying temperature in the step (2) is 70-90 ℃, and the drying time is 8-12 h.
In a second aspect, the invention provides the high-thermal-conductivity and high-thermal-stability three-phase fluorescent ceramic for laser illumination prepared by the preparation method, wherein the three-phase fluorescent ceramic is Ce: luAG-MgAl 2 O 4 MgO, ce: luAG as ceramic host, mgAl 2 O 4 And MgO are both highly thermally conductive phases.
The fluorescent ceramic emits high-brightness broadband yellow light near 550nm under the excitation of a blue light LD chip with the wavelength near 455nm, and the thermal conductivity is 28Wm -1 K -1 ～32Wm -1 K -1 The emission intensity only loses 1.4% -3.4% at 150 ℃, and only loses 3.2% -5.8% at 250 ℃.
The prepared multiphase ceramic material adopts Ce: luAG as a main phase, and excessive MgO is added to react with partial LuAG at a specific temperature to generate MgAl while being used as a sintering aid 2 O 4 And Lu 2 O 3 Very small proportion of MgAl during the temperature rise 2 O 4 And Lu 2 O 3 Re-reacting to generate Lu (Al, mg) O 3 Most of MgAl 2 O 4 The composite phase is taken as LuAG complex phase together with MgO, and the heat conductivity is obviously improved and the light scattering effect and the light absorption rate are effectively enhanced by regulating the content of the MgO.
Compared with the prior art, the invention has the following beneficial effects:
(1) The three-phase ceramic prepared by the invention can emit high-brightness broadband yellow light near 550nm under the excitation of a blue light LD chip with the wavelength near 455 nm.
(2) The invention fully utilizes the advantage of excessive addition of MgO, and the MgO is reacted with LuAG to generate MgAl while being used as a sintering aid 2 O 4 The composite phase is taken as LuAG complex phase together with MgO, and the thermal conductivity and the thermal stability of the composite phase are obviously improved.
(3) The invention adopts Ce of LuAG-MgAl 2 O 4 Three phases of MgO, by MgAl 2 O 4 And the introduction of an MgO two-phase scattering source improves the utilization rate of blue light, relieves the total reflection (TIR) effect of fluorescence and effectively improves the light extraction rate.
(4) The Ce, luAG-MgAl with high brightness and high thermal stability is prepared by SPS sintering 2 O 4 the-MgO three-phase ceramic has simple preparation method and short time, can be applied to high-power LED/LDs devices, and greatly improves the application value of the devices.
Drawings
FIG. 1 shows that the sample Ce: luAG-MgAl prepared in example 1 of the present invention 2 O 4 -XRD pattern of MgO: (A) LuAG, mgO and sample comparison chart, (B) MgAl 2 O 4 Comparison with samples;
FIG. 2 shows that the sample Ce: luAG-MgAl prepared in example 1 of the present invention 2 O 4 -EL spectrum of MgO under LD chip excitation at 455 nm;
FIG. 3 is a sample Ce: luAG-MgAl prepared in examples 1 to 4 of the present invention 2 O 4 A variable temperature spectrogram of MgO accounting for 20-50% of the total mass of the Ce, the LuAG and the MgO;
FIG. 4 is a sample Ce: luAG-MgAl prepared in examples 1 to 4 of the present invention 2 O 4 -MgO, mgO accounts for 20% -50% of the total mass of both Ce: luAG and MgO.
Detailed Description
The invention is described in further detail below with reference to the figures and specific examples.
The Ce, luAG powder and MgO powder used in the following examples are commercially available products.
Example 1
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 30 percent of the total mass of Ce, luAG and MgO, and 42g of Ce, luAG powder with the purity of 99.99 percent and the grain diameter of 1.2 mu m and 18g of MgO powder with the purity of 99.99 percent and the grain diameter of 1.7 mu m are respectively weighed according to the stoichiometric ratio of corresponding raw materials. Mixing Ce, luAG and MgO, adding absolute ethyl alcohol, ball milling and fully mixingAnd mixing, drying the powder obtained after ball milling in an oven at 90 ℃ for 12h to obtain dry powder, wrapping the dry powder with graphite paper, and then performing discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1550 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 32Wm -1 K -1 The emission intensity lost only 1.4% at 150 ℃ and only 3.2% at 250 ℃.
Example 2
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 20 percent of the total mass of the Ce, the LuAG and the MgO, and according to the stoichiometric ratio of corresponding raw materials, 48g of Ce, luAG powder with the purity of 99.99 percent and the grain diameter of 1.2 mu m and 12g of MgO with the purity of 99.99 percent and the grain diameter of 1.7 mu m are respectively weighed. The preparation method comprises the steps of blending Ce, luAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying powder obtained after ball milling in an oven at 90 ℃ for 12 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1550 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 28.8Wm -1 K -1 The emission intensity lost only 3.2% at 150 ℃ and only 5.2% at 250 ℃.
Example 3
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 40 percent of the total mass of the Ce, the LuAG and the MgO, and according to the stoichiometric ratio of corresponding raw materials, 36g of the Ce with the purity of 99.99 percent and the grain diameter of 1.2 mu m and 24g of the MgO with the purity of 99.99 percent and the grain diameter of 1.7 mu m are respectively weighed. Mixing Ce, luAG and MgO, adding absolute ethyl alcohol, ball-milling and fully mixing, drying the powder obtained after ball-milling in an oven at 90 ℃ for 12h to obtain dry powder, and using the dry powderAnd (3) after wrapping the graphite paper, performing discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1550 ℃, and cooling to room temperature to obtain the three-phase ceramic. Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 30Wm -1 K -1 The emission intensity lost only 2.4% at 150 ℃ and only 3.8% at 250 ℃.
Example 4
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 50 percent of the total mass of Ce, luAG and MgO, and 30g of Ce, luAG with the purity of 99.99 percent and the grain diameter of 1.2 mu m and 30g of MgO with the purity of 99.99 percent and the grain diameter of 1.7 mu m are respectively weighed according to the stoichiometric ratio of corresponding raw materials. The preparation method comprises the steps of blending Ce, luAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying powder obtained after ball milling in an oven at 90 ℃ for 12 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1550 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 28Wm -1 K -1 The emission intensity lost only 3.4% at 150 ℃ and only 5.8% at 250 ℃.
FIG. 3 is a sample Ce: luAG-MgAl prepared in examples 1 to 4 of the present invention 2 O 4 -MgO, wherein MgO accounts for 20% -50% of the total mass of the Ce to the LuAG and the MgO. As can be seen from FIG. 3, the loss of emission intensity at 150 ℃ ranged between 1.4% and 3.4%, and the loss of emission intensity at 250 ℃ ranged between 3.2% and 5.8%.
FIG. 4 is a sample Ce: luAG-MgAl prepared in examples 1 to 4 of the present invention 2 O 4 -MgO, mgO accounts for 20% -50% of the total mass of both Ce: luAG and MgO. As can be seen from FIG. 4, the thermal conductivity was 28Wm -1 K -1 -32Wm -1 K -1 In the meantime.
Example 5
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 30 percent of the total mass of Ce, luAG and MgO, and according to the stoichiometric ratio of corresponding raw materials, 42g of Ce with the purity of 99.99 percent and the grain diameter of 1 mu m, and 18g of MgO with the purity of 99.99 percent and the grain diameter of 1.5 mu m are respectively weighed. The preparation method comprises the steps of blending Ce, luAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying powder obtained after ball milling in an oven at 70 ℃ for 9 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 50MPa, the pulse current is 200A, the heat preservation sintering time is 50min, the sintering temperature is 1500 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 29.7Wm -1 K -1 The emission intensity lost only 2.1% at 150 ℃ and only 4% at 250 ℃.
Example 6
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, 30 percent of MgO accounts for the total mass of Ce, luAG and MgO, and 42g of Ce, luAG and 18g of MgO with the purity of 99.99 percent and the grain diameter of 1.3 mu m and the grain diameter of 2 mu m are respectively weighed according to the stoichiometric ratio of the corresponding raw materials. Mixing the Ce, namely LuAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying the powder obtained after ball milling in an oven at the temperature of 80 ℃ for 9 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 100MPa, the pulse current is 400A, the heat preservation sintering time is 20min, the sintering temperature is 1480 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 30.2Wm -1 K -1 The emission intensity lost only 1.8% at 150 ℃ and only 3.7% at 250 ℃.
Example 7
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, 30 percent of MgO accounts for the total mass of Ce, luAG and MgO, and according to the stoichiometric ratio of corresponding raw materials, 42g of Ce, luAG with the purity of 99.99 percent and the grain diameter of 1.2 mu m and 18g of MgO with the purity of 99.99 percent and the grain diameter of 1.8 mu m are respectively weighed. The preparation method comprises the steps of blending Ce, luAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying powder obtained after ball milling in an oven at 90 ℃ for 12 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1580 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 29.8Wm -1 K -1 The emission intensity lost only 1.6% at 150 ℃ and only 3.2% at 250 ℃.
Example 8
According to the chemical formula Ce: luAG-MgAl 2 O 4 In the MgO, mgO accounts for 30 percent of the total mass of Ce, luAG and MgO, and according to the stoichiometric ratio of corresponding raw materials, 42g of Ce, luAG with the purity of 99.99 percent and the grain diameter of 1.1 mu m, 18g of MgO with the purity of 99.99 percent and the grain diameter of 1.5 mu m, 1.1 mu m of Ce. The preparation method comprises the steps of blending Ce, luAG and MgO, adding absolute ethyl alcohol, carrying out ball milling, fully mixing, drying powder obtained after ball milling in an oven at 90 ℃ for 12 hours to obtain dry powder, wrapping the dry powder with graphite paper, carrying out discharge plasma sintering in a vacuum state, wherein the sintering pressure is 80MPa, the pulse current is 300A, the heat preservation sintering time is 40min, the sintering temperature is 1600 ℃, and cooling to room temperature to obtain the three-phase ceramic.
Under the excitation of a blue light LD chip with the wavelength of about 455nm, high-brightness broadband yellow light with the wavelength of about 550nm is emitted, and the thermal conductivity is 30.3Wm -1 K -1 The emission intensity lost only 1.8% at 150 ℃ and only 3.4% at 250 ℃.
The above description is only for the purpose of illustrating the embodiments of the present invention, and the scope of the present invention should not be limited thereto, and any modifications, equivalents and improvements made by those skilled in the art within the technical scope of the present invention as disclosed in the present invention should be covered by the scope of the present invention.
Claims (6)
1. A preparation method of a three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination is characterized by comprising the following steps:
(1) Respectively weighing Ce, luAG powder and MgO powder according to the mass ratio to serve as ceramic raw material powder, wherein MgO accounts for 20-50% of the total mass of the ceramic raw material powder;
(2) Mixing the Ce, luAG and MgO, adding absolute ethyl alcohol, and fully mixing by ball milling;
(3) Taking out and drying the slurry obtained after ball milling to obtain dry powder;
(4) And (3) wrapping the dried powder with graphite paper, then performing discharge plasma sintering in a vacuum state, and cooling to room temperature to obtain the three-phase fluorescent ceramic.
2. The method for preparing the three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination according to claim 1, wherein the particle size of the Ce: luAG powder in the step (1) is 1-1.3 μm, the particle size of the MgO powder is 1.5-2 μm, and the purity is more than 99.99%.
3. The method for preparing the three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination according to claim 1, wherein the sintering pressure of the spark plasma sintering in the step (4) is 50-100 MPa, the pulse current is 200-400A, the heat preservation sintering time is 20-50 min, and the sintering temperature is 1480-1600 ℃.
4. The preparation method of the three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination according to claim 1, wherein the ball milling rotation speed in the step (2) is 180-250 rpm, and the ball milling time is 15-30 h.
5. The method for preparing the three-phase fluorescent ceramic with high thermal conductivity and high thermal stability for laser illumination according to claim 1, wherein the drying temperature in the step (2) is 70-90 ℃ and the drying time is 8-12 h.
6. The high-thermal-conductivity high-thermal-stability three-phase fluorescent ceramic for laser lighting, prepared by the preparation method according to any one of claims 1 to 5.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN116425544A (en) * | 2023-04-20 | 2023-07-14 | 江苏师范大学 | High-brightness high-luminous-efficiency complex-phase fluorescent ceramic for laser illumination and preparation method thereof |
| CN116444271A (en) * | 2023-05-06 | 2023-07-18 | 江苏师范大学 | High-color-rendering-index high-thermal-stability fluorescent ceramic for LD/LED and preparation method thereof |
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| CN116444271A (en) * | 2023-05-06 | 2023-07-18 | 江苏师范大学 | High-color-rendering-index high-thermal-stability fluorescent ceramic for LD/LED and preparation method thereof |
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