CN108610038B - Method for preparing YAG transparent ceramic by zirconium oxide and YAG powder double-layer embedding sintering - Google Patents

Method for preparing YAG transparent ceramic by zirconium oxide and YAG powder double-layer embedding sintering Download PDF

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CN108610038B
CN108610038B CN201810492985.2A CN201810492985A CN108610038B CN 108610038 B CN108610038 B CN 108610038B CN 201810492985 A CN201810492985 A CN 201810492985A CN 108610038 B CN108610038 B CN 108610038B
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yag
powder
sintering
transparent ceramic
biscuit
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CN108610038A (en
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张乐
蒋志刚
顾灵诚
姚庆
周天元
高光珍
王骋
陈浩
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Jiangsu Normal University
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    • C04B35/48—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on zirconium or hafnium oxides, zirconates, zircon or hafnates
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Abstract

The invention discloses a method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconium oxide and YAG powder, which comprises the steps of pumping ammonium bicarbonate solution into a mixed solution of yttrium ions and aluminum ions, aging, washing, drying and sieving to obtain a precursor, calcining, ball-milling, sieving, dry-pressing and forming, cold isostatic pressing to obtain a YAG biscuit, embedding the YAG biscuit according to the arrangement mode of zirconium oxide powder-YAG biscuit-YAG powder-zirconium oxide powder, and then sequentially carrying out vacuum sintering and grinding and polishing treatment to obtain the YAG transparent ceramic. According to the invention, the zirconia powder can provide oxygen ions for the YAG powder and the YAG biscuit during vacuum sintering, so that the generation of oxygen vacancies in the YAG ceramic in the sintering stage can be effectively inhibited, the reduction of the transmittance of the YAG transparent ceramic is prevented, the annealing step is omitted, and the energy-saving and environment-friendly effects are achieved.

Description

Method for preparing YAG transparent ceramic by zirconium oxide and YAG powder double-layer embedding sintering
Technical Field
The invention belongs to the technical field of transparent ceramic preparation, and particularly relates to a method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder.
Background
The YAG transparent ceramic has the characteristics of high strength, good heat resistance and strong corrosion resistance, and has good permeability to visible light and infrared light, and the properties enable the YAG transparent ceramic to be applied to the fields of high-pressure gas lamp tubes, high-temperature window materials, laser ceramics, scintillating ceramics and the like. Therefore, the YAG transparent ceramic prepared has wide application prospect and is one of the hot spots of material science research.
In the conventional process of preparing transparent ceramics, the most common sintering method is vacuum sintering. Compared with other sintering modes (such as hot isostatic pressing and spark plasma sintering), the vacuum sintering has the characteristics of high efficiency, energy conservation and the like. However, there are many problems in the vacuum sintering process, such as the color of the YAG transparent ceramic becomes grey after vacuum sintering. The reason is mainly because oxygen ions in the YAG ceramic can escape due to the oxygen-deficient condition in the vacuum furnace during the vacuum sintering process, thereby generating oxygen vacancies. In order to solve this problem, in many cases, researchers have conducted long-term (10 hours or more) air or oxygen atmosphere annealing on YAG ceramics after vacuum sintering to eliminate oxygen vacancies. However, after annealing, since impurities such as carbon, sulfur, etc. remaining inside the ceramic are removed at the annealing stage, some nano-pores are left, which severely reduce the transmittance of the transparent ceramic.
Disclosure of Invention
The invention aims to provide a method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder, wherein the YAG transparent ceramic after vacuum sintering has no color graying phenomenon, the transmittance of the ceramic is obviously improved, and subsequent annealing is not needed.
In order to achieve the purpose, the invention adopts the following technical scheme:
a method for preparing YAG transparent ceramic by zirconium oxide and YAG powder double-layer embedding sintering comprises the following steps:
1) preparing a precursor: preparing an yttrium nitrate solution with the concentration of 0.1-0.3 mol/L, adding ammonium aluminum sulfate dodecahydrate crystals into the yttrium nitrate solution, and uniformly stirring to form a mixed solution, wherein the molar ratio of yttrium ions to aluminum ions is 3: 5; pumping an ammonium bicarbonate solution with the concentration of 1.5-2 mol/L into the mixed solution by using a peristaltic pump under the stirring state; monitoring the pH value of the reaction system, stopping pumping and stirring when the pH value reaches 8.0-8.2, standing and aging the reaction system for 12-24 h, and sequentially washing, filtering and drying the aged precursor to obtain precursor powder;
2) and (3) calcining: sieving the precursor powder obtained in the step 1), and calcining the sieved precursor powder in a muffle furnace at 1100-1300 ℃ for 2-4 h to obtain nano YAG powder;
3) ball milling: adding 0.4-0.6 wt.% of tetraethoxysilane into the nano YAG powder obtained in the step 2), adding absolute ethyl alcohol and high-purity alumina grinding balls, performing ball milling and mixing to obtain slurry, drying the slurry, and performing screening treatment;
4) molding: putting the powder sieved in the step 3) into a die, forming a round YAG biscuit by adopting a dry pressing method, and then carrying out cold isostatic pressing treatment;
5) and (3) sintering: placing the YAG biscuit obtained in the step 4) in a muffle furnace for biscuit firing, and removing residual organic matters; then placing the bisque-fired YAG biscuit in a tungsten crucible A, and embedding according to the arrangement mode of zirconia powder-YAG biscuit-YAG powder-zirconia powder; after embedding, reversely buckling a tungsten crucible B with a slightly larger caliber above the tungsten crucible A to prevent powder from being pumped away by a mechanical pump or a molecular pump, and then putting the tungsten crucible B into a vacuum sintering furnace for vacuum sintering;
6) grinding and polishing: and grinding and polishing the two sides of the ceramic wafer subjected to vacuum sintering to 1-3 mm to obtain the YAG transparent ceramic.
Preferably, when the ammonium bicarbonate solution is pumped in the step (1), the pumping speed is 1-6 mL/min, and the stirring speed is 300-500 rpm.
Preferably, the washing in the step (1) is carried out for 2-4 times by using deionized water, and then is carried out for 2-4 times by using absolute ethyl alcohol; the drying temperature is 40-60 ℃, and the drying time is 12-36 h.
Preferably, the sieve mesh used in the step (2) has a size of 100-200 meshes, and the sieving frequency is 3-5 times.
Preferably, in the step (3), the ball milling rotation speed is 160-200 rpm, the ball milling time is 12-24 hours, the drying temperature is 40-60 ℃, the drying time is 12-36 hours, the size of the screen is 100-200 meshes, and the screening frequency is 3-5 times.
Preferably, the dry pressing pressure in the step (4) is 25-35 MPa, the pressure maintaining time is 1-3 min, and the diameter of the round YAG biscuit is 16-30 mm; the pressure of the cold isostatic pressing is 200-240 Mpa, and the pressure maintaining time is 4-8 min.
Preferably, in the step (5), the bisque firing temperature is 800-900 ℃, and the bisque firing time is 5-8 hours; the degree of vacuum in the vacuum sintering furnace was 1.0X 10-5～1.0×10-3Pa, the vacuum sintering temperature is 1760-1800 ℃, and the sintering time is 8-20 h.
Preferably, the thickness ratio of the zirconium oxide powder layer to the YAG green body during the embedding in the step (5) is 1.0-3.0, and the thickness ratio of the YAG powder layer to the YAG green body is 3.0-4.0.
Preferably, the inner diameter of the tungsten crucible B is 1.2 to 2.0 times the outer diameter of the tungsten crucible A.
The invention adopts a coprecipitation method to prepare YAG transparent ceramics, and adopts zirconium oxide and YAG double-layer powder to embed ceramic biscuit in the vacuum sintering stage, thereby inhibiting the generation of oxygen vacancy and improving the optical quality of the YAG transparent ceramics.
Compared with the prior art, the invention has the following beneficial effects:
(1) in the vacuum sintering stage, zirconium oxide and YAG powder in a certain proportion are adopted, a biscuit is embedded in a mode of zirconium oxide powder-YAG biscuit-YAG powder-zirconium oxide powder, and then vacuum sintering is carried out in a vacuum sintering furnace. Because the zirconia powder can provide oxygen ions to the YAG powder and the YAG biscuit during vacuum sintering, the generation of oxygen vacancies in the sintering stage can be effectively inhibited, and the reduction of the transmittance of the YAG ceramic can be prevented.
(2) Since the generation of oxygen vacancies is suppressed at the vacuum sintering stage, a conventional annealing process is not required, and the generation of nano-pores left by the removal of impurities such as carbon, sulfur, etc. remaining in the ceramic during the annealing process is reduced. And because the step of annealing is omitted, the method is more energy-saving and environment-friendly, and has a great promoting effect on the batch production of YAG ceramics.
Drawings
FIG. 1 is a diagram of an apparatus of the present invention;
FIG. 2 is a diagram of an apparatus according to a comparative example of the present invention.
In the figure, a 1-tungsten crucible A, a 2-zirconia powder layer, a 3-YAG powder layer, a 4-YAG biscuit and a 5-tungsten crucible B are arranged.
FIG. 3 is a diagram showing a transparent ceramic sample obtained in example 1 of the present invention.
In the figure, (a) is a transparent ceramic sample after vacuum sintering, and (b) is a transparent ceramic sample after direct grinding and polishing.
FIG. 4 is a diagram showing a transparent ceramic sample obtained by a comparative example of the present invention.
In the figure, (a) is a transparent ceramic sample after vacuum sintering, and (b) is a transparent ceramic sample after annealing, grinding and polishing.
Detailed Description
The invention is further illustrated with reference to the following figures and specific examples, which should not be construed as limiting the scope of the invention.
Example 1: d (ZrO)2) YAG transparent ceramics prepared by 1.0 percent of d (YAG biscuit)
Pouring Y (NO) into the container3)3·6H2Diluting O crystal with deionized water to obtain Y (NO)3)3Solution, Y3+The solution concentration is 0.1mol/L, NH is added into yttrium nitrate solution4Al(SO4)2·12H2Crystal of O, assurance of Y3+With Al3+The molar ratio is 3:5, the mixture is stirred uniformly by a stirrer, and the stirring speed is 300rpm, so that a mixed solution is formed; NH with the concentration of 1.5mol/L is pumped by a peristaltic pump under the stirring state4HCO3Pumping into the mixed solution, wherein the manner of pumping the precipitator into the mixed solution is spraying, and the pumping rate is 1 mL/min; and measuring the pH value of the reaction system by using a pH meter, stopping pumping and stirring when the pH value reaches 8.0, and standing and aging the reaction system for 12 hours. Washing the aged precursor with deionized water for 2 times, then washing with absolute ethyl alcohol for 2 times, and after the filtration is finished, putting the obtained precursor into an oven for drying, wherein the drying temperature is 40 ℃, and the drying time is 12 hours.
And (4) sieving the dried precursor powder for 5 times with a sieve of 100 meshes. And (4) placing the sieved powder into a muffle furnace to be calcined for 2 hours at 1100 ℃ to obtain the nano YAG powder.
And adding 0.4 wt.% of TEOS into the calcined powder, adding absolute ethyl alcohol and high-purity alumina grinding balls, and carrying out ball milling and mixing, wherein the ball milling rotation speed is 160rpm, and the ball milling time is 12 hours. And then, putting the slurry into an oven for drying at 40 ℃ for 12h, and then sieving for 5 times with a sieve of 100 meshes.
And carrying out dry pressing molding on the obtained powder, wherein the dry pressing pressure is 25MPa, the pressure maintaining time is 1min, and the powder is pressed into a round biscuit with the diameter of 16 mm. Then cold isostatic pressing treatment is carried out, the pressure of the cold isostatic pressing is 200Mpa, and the pressure maintaining time is 4 min.
Placing the biscuit in a muffle furnace, and biscuiting for 5 hours at 800 ℃ to remove residual organic matters; as shown in fig. 1, the biscuit after firing was placed in a tungsten crucible a1 and embedded in a manner of zirconia powder-YAG biscuit-YAG powder-zirconia powder, wherein the thickness ratio of the zirconia powder layer 2 used for the cladding to the YAG biscuit 4 was 1.0, and the thickness ratio of the YAG powder layer 3 to the YAG biscuit 4 was 3.0. A tungsten crucible B5 with a slightly larger caliber is reversely buckled above the tungsten crucible A1 to prevent the powder from being pumped away by a mechanical pump or a molecular pump, wherein the inner diameter of the tungsten crucible B5 is 1.2 times of the outer diameter of the tungsten crucible A1. Then placing the mixture into a vacuum sintering furnace for vacuum sintering, wherein the vacuum degree in the vacuum sintering furnace is 1.0 multiplied by 10-5Pa, the vacuum sintering temperature is 1760 ℃, and the sintering time is 20 h. In the vacuum sintering process, the zirconia powder can provide oxygen ions for the YAG powder and the YAG biscuit, so that the generation of oxygen vacancies in the ceramic can be effectively inhibited. Therefore, the YAG transparent ceramic after vacuum sintering does not generate the phenomenon of grey color, further annealing is not needed, and the high optical quality of the transparent ceramic can be ensured. FIG. 3(a) is a YAG transparent ceramic sample after vacuum sintering, and it can be seen that the sample after vacuum sintering has no graying phenomenon, which indicates that almost no oxygen vacancy is generated in the ceramic during the vacuum sintering stage, and no further annealing is needed.
And directly grinding and polishing the two sides of the ceramic wafer subjected to vacuum sintering to 1mm to obtain the YAG transparent ceramic. FIG. 3(b) shows a polished YAG transparent ceramic sample, which shows almost no scattering points inside the transparent ceramic and has high optical quality.
Example 2: d (ZrO)2) Preparing YAG transparent ceramic by using 2.0% of d (YAG biscuit)
Pouring Y (NO) into the container3)3·6H2Diluting O crystal with deionized water to obtain Y (NO)3)3Solution, Y3+The solution concentration is 0.2mol/L, NH is added into yttrium nitrate solution4Al(SO4)2·12H2Crystal of O, assurance of Y3+With Al3+The molar ratio is 3:5, the mixture is stirred uniformly by a stirrer, and the stirring speed is 400rpm, so that a mixed solution is formed; NH with the concentration of 1.8mol/L is pumped by a peristaltic pump under the stirring state4HCO3Pumping into the mixed solution, wherein the manner of pumping the precipitator into the yttrium nitrate solution is spraying, and the pumping rate is 2 mL/min; and measuring the pH value of the reaction system by using a pH meter, stopping pumping and stirring when the pH value reaches 8.1, and standing and aging the reaction system for 16 hours. Washing the aged precursor with deionized water for 3 times, then washing with absolute ethyl alcohol for 3 times, and after the filtration is finished, putting the obtained precursor into an oven for drying at the drying temperature of 50 ℃ for 24 hours.
And (4) sieving the dried precursor powder for 4 times with a sieve of 150 meshes. And after sieving, putting the powder into a muffle furnace to calcine the powder for 3 hours at 1200 ℃ to obtain the nano YAG powder.
And adding 0.5 wt.% TEOS into the calcined powder, adding absolute ethyl alcohol and high-purity alumina grinding balls, and carrying out ball milling and mixing, wherein the ball milling rotation speed is 180rpm, and the ball milling time is 20 hours. And then, putting the slurry into an oven for drying at 50 ℃ for 20h, and then sieving for 4 times with a sieve of 150 meshes.
And carrying out dry pressing molding on the obtained powder, wherein the dry pressing pressure is 30MPa, the pressure maintaining time is 2min, and the powder is pressed into a round biscuit with the diameter of 20 mm. And then carrying out cold isostatic pressing treatment, wherein the pressure of the cold isostatic pressing is 220Mpa, and the pressure maintaining time is 5 min.
Placing the biscuit in a muffle furnace, and biscuiting for 6 hours at 850 ℃ to remove residual organic matters; as shown in FIG. 1, the biscuit after firing was placed in a tungsten crucible A1 and embedded in a manner of zirconia powder-YAG biscuit-YAG powder-zirconia powder, wherein the thickness ratio of the zirconia powder layer 2 used for the cladding layer to the YAG biscuit 4 was 2.0, and the YAG powder layer was formed by coatingThe thickness ratio of 3 to YAG biscuit 4 is 3.5. A tungsten crucible B5 with a slightly larger diameter is reversely buckled above the tungsten crucible A1 to prevent the powder from being pumped away by a mechanical pump or a molecular pump, wherein the inner diameter of the tungsten crucible B5 is 1.5 times of the outer diameter of the tungsten crucible A1. Then placing the mixture into a vacuum sintering furnace for vacuum sintering, wherein the vacuum degree in the vacuum sintering furnace is 1.0 multiplied by 10-4Pa, the vacuum sintering temperature is 1780 ℃, and the sintering time is 16 h. In the vacuum sintering process, the zirconia powder can provide oxygen ions for the YAG powder and the YAG biscuit, so that the generation of oxygen vacancies in the ceramic can be effectively inhibited. Therefore, the YAG transparent ceramic after vacuum sintering has no color and ash phenomenon, further annealing is not needed, and the high optical quality of the transparent ceramic is ensured.
And grinding and polishing the two sides of the ceramic wafer subjected to vacuum sintering to 1.2mm to obtain the YAG transparent ceramic.
Example 3: d (ZrO)2) Preparing YAG transparent ceramic by using 3.0 g of d (YAG biscuit)
Pouring Y (NO) into the container3)3·6H2Diluting O crystal with deionized water to obtain Y (NO)3)3Solution, Y3+The solution concentration is 0.3mol/L, NH is added into yttrium nitrate solution4Al(SO4)2·12H2Crystal of O, assurance of Y3+With Al3+The molar ratio is 3:5, the mixture is stirred uniformly by a stirrer, and the stirring speed is 500rpm, so that a mixed solution is formed; under the stirring state, NH with the concentration of 2mol/L is pumped by a peristaltic pump4HCO3Pumping into the mixed solution, wherein the manner of pumping the precipitator into the yttrium nitrate solution is spraying, and the pumping rate is 6 mL/min; and measuring the pH value of the reaction system by using a pH meter, stopping pumping and stirring when the pH value reaches 8.2, and standing and aging the reaction system for 20 hours. Washing the aged precursor with deionized water for 4 times, then washing with absolute ethyl alcohol for 4 times, and after the filtration is finished, putting the obtained precursor into an oven for drying, wherein the drying temperature is 60 ℃, and the drying time is 36 h.
And (4) sieving the dried precursor powder for 3 times with a 200-mesh sieve. And (4) after sieving, putting the mixture into a muffle furnace to calcine for 4 hours at 1300 ℃ to obtain the nano YAG powder.
And adding 0.6 wt.% TEOS into the calcined powder, adding absolute ethyl alcohol and high-purity alumina grinding balls, and carrying out ball milling and mixing, wherein the ball milling rotation speed is 200rpm, and the ball milling time is 24 hours. And then, drying the slurry in an oven at 60 ℃ for 36h, and then sieving the slurry for 3 times with a 200-mesh sieve.
And carrying out dry pressing molding on the obtained powder, wherein the dry pressing pressure is 35MPa, the pressure maintaining time is 3min, and the powder is pressed into a round biscuit with the diameter of 30 mm. Then cold isostatic pressing is carried out, the pressure of the cold isostatic pressing is 240Mpa, and the pressure maintaining time is 8 min.
Placing the biscuit in a muffle furnace, and biscuiting for 8 hours at 900 ℃ to remove residual organic matters; as shown in fig. 1, the biscuit after firing was placed in a tungsten crucible a1 and embedded in a manner of zirconia powder-YAG biscuit-YAG powder-zirconia powder, wherein the thickness ratio of the zirconia powder layer 2 used for the cladding to the YAG biscuit 4 was 3.0, and the thickness ratio of the YAG powder layer 3 to the YAG biscuit 4 was 4.0. A tungsten crucible B5 with a slightly larger diameter is reversely buckled above the tungsten crucible A1 to prevent the powder from being pumped away by a mechanical pump or a molecular pump, wherein the inner diameter of the tungsten crucible B5 is 2.0 times of the outer diameter of the tungsten crucible A1. Then placing the mixture into a vacuum sintering furnace for vacuum sintering, wherein the vacuum degree in the vacuum sintering furnace is 1.0 multiplied by 10-3Pa, the vacuum sintering temperature is 1800 ℃ and the sintering time is 20 h. In the vacuum sintering process, the zirconia powder can provide oxygen ions for the YAG powder and the YAG biscuit, so that the generation of oxygen vacancies in the ceramic can be effectively inhibited. Therefore, the YAG transparent ceramic after vacuum sintering has no color and ash phenomenon, further annealing is not needed, and the high optical quality of the transparent ceramic is ensured.
And grinding and polishing the two sides of the ceramic wafer after vacuum sintering to 3mm to obtain the YAG transparent ceramic.
Comparative example: preparation of YAG transparent ceramic by single-layer YAG powder embedding
Pouring Y (NO) into the container3)3·6H2Diluting O crystal with deionized water to obtain Y (NO)3)3Solution, Y3+The solution concentration is 0.1mol/L, NH is added into yttrium nitrate solution4Al(SO4)2·12H2Crystal of O, assurance of Y3+With Al3+The molar ratio is 3:5, the mixture is stirred uniformly by a stirrer, and the stirring speed is 300rpm, so that a mixed solution is formed; NH with the concentration of 1.5mol/L is pumped by a peristaltic pump under the stirring state4HCO3Pumping into the mixed solution, wherein the manner of pumping the precipitator into the mixed solution is spraying, and the pumping rate is 1 mL/min; and measuring the pH value of the reaction system by using a pH meter, stopping pumping and stirring when the pH value reaches 8.0, and standing and aging the reaction system for 12 hours. Washing the aged precursor with deionized water for 2 times, then washing with absolute ethyl alcohol for 2 times, and after the filtration is finished, putting the obtained precursor into an oven for drying, wherein the drying temperature is 40 ℃, and the drying time is 12 hours.
And (4) sieving the dried precursor powder for 5 times with a sieve of 100 meshes. And (4) placing the sieved powder into a muffle furnace to be calcined for 2 hours at 1100 ℃ to obtain the nano YAG powder.
And adding 0.4 wt.% of TEOS into the calcined powder, adding absolute ethyl alcohol and high-purity alumina grinding balls, and carrying out ball milling and mixing, wherein the ball milling rotation speed is 160rpm, and the ball milling time is 12 hours. And then, putting the slurry into an oven for drying at 40 ℃ for 12h, and then sieving for 5 times with a sieve of 100 meshes.
And carrying out dry pressing molding on the obtained powder, wherein the dry pressing pressure is 25MPa, the pressure maintaining time is 1min, and the powder is pressed into a round biscuit with the diameter of 16 mm. Then cold isostatic pressing treatment is carried out, the pressure of the cold isostatic pressing is 200Mpa, and the pressure maintaining time is 4 min.
Placing the biscuit in a muffle furnace, and biscuiting for 5 hours at 800 ℃ to remove residual organic matters; as shown in fig. 2, the biscuit after firing was placed in a tungsten crucible a1 and embedded in a YAG powder-YAG biscuit-YAG powder system, wherein the thickness ratio of the cladding YAG powder layer 3 to the YAG biscuit 4 was 3.0. A tungsten crucible B5 with a slightly larger caliber is reversely buckled above the tungsten crucible A1 to prevent the powder from being pumped away by a mechanical pump or a molecular pump, wherein the inner diameter of the tungsten crucible B5 is 1.2 times of the outer diameter of the tungsten crucible A1. Then placing the mixture in a vacuum sintering furnace for vacuum sintering. The degree of vacuum in the vacuum sintering furnace was 1.0X 10-5Pa, the vacuum sintering temperature is 1760 ℃, and the sintering time is 20h. Because zirconia powder is not used for embedding, an oxygen-rich environment for providing oxygen ions for the YAG biscuit is lacked in the sintering process, and therefore, the ceramic surface after vacuum sintering generates a phenomenon of grey color and needs to be subjected to further annealing operation. FIG. 4(a) is a YAG transparent ceramic sample after vacuum sintering, which shows that the sample after vacuum sintering has serious graying phenomenon, and illustrates that the ceramic generates serious oxygen vacancy phenomenon after vacuum sintering and needs further annealing.
And annealing the vacuum sintered ceramic at 1450 ℃ for 10 h. And (4) after annealing, carrying out double-sided grinding and polishing on the ceramic wafer to 1mm to obtain the YAG transparent ceramic. FIG. 4(b) shows a polished transparent ceramic sample, in which a large amount of "haze" exists in the transparent ceramic, and the optical quality is not high. This is because impurities such as carbon and sulfur remaining in the ceramic after vacuum sintering are removed during annealing, thereby causing voids and resulting in poor optical quality.

Claims (9)

1. A method for preparing YAG transparent ceramic by zirconium oxide and YAG powder double-layer embedding sintering is characterized by comprising the following steps:
1) preparing a precursor: preparing an yttrium nitrate solution with the concentration of 0.1-0.3 mol/L, adding ammonium aluminum sulfate dodecahydrate crystals into the yttrium nitrate solution, and uniformly stirring to form a mixed solution, wherein the molar ratio of yttrium ions to aluminum ions is 3: 5; pumping an ammonium bicarbonate solution with the concentration of 1.5-2 mol/L into the mixed solution by using a peristaltic pump under the stirring state; monitoring the pH value of the reaction system, stopping pumping and stirring when the pH value reaches 8.0-8.2, standing and aging the reaction system for 12-24 h, and sequentially washing, filtering and drying the aged precursor to obtain precursor powder;
2) and (3) calcining: sieving the precursor powder obtained in the step 1), and calcining the sieved precursor powder in a muffle furnace at 1100-1300 ℃ for 2-4 h to obtain nano YAG powder;
3) ball milling: adding 0.4-0.6 wt.% of tetraethoxysilane into the nano YAG powder obtained in the step 2), adding absolute ethyl alcohol and alumina grinding balls, performing ball milling and mixing to obtain slurry, drying the slurry, and performing screening treatment;
4) molding: putting the powder sieved in the step 3) into a die, forming a round YAG biscuit by adopting a dry pressing method, and then carrying out cold isostatic pressing treatment;
5) and (3) sintering: placing the YAG biscuit obtained in the step 4) in a muffle furnace for biscuit firing, and removing residual organic matters; then placing the bisque-fired YAG biscuit in a tungsten crucible A (1), and embedding according to the arrangement mode of zirconia powder-YAG biscuit-YAG powder-zirconia powder; after embedding, reversely buckling a tungsten crucible B (5) with a slightly larger caliber above the tungsten crucible A (1), and then putting the tungsten crucible B into a vacuum sintering furnace for vacuum sintering;
6) grinding and polishing: and grinding and polishing the two sides of the ceramic wafer subjected to vacuum sintering to 1-3 mm to obtain the YAG transparent ceramic.
2. The method for preparing YAG transparent ceramic by double-layer embedding and sintering of zirconia and YAG powder according to claim 1, wherein the pumping rate of the ammonium bicarbonate solution in the step (1) is 1-6 mL/min, and the stirring speed is 300-500 rpm.
3. The method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder according to claim 1 or 2, wherein the washing in step (1) is washing with deionized water for 2-4 times, and then washing with absolute ethanol for 2-4 times; the drying temperature is 40-60 ℃, and the drying time is 12-36 h.
4. The method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder according to claim 1 or 2, wherein the sieve mesh used in step (2) is 100-200 mesh, and the sieving frequency is 3-5 times.
5. The method for preparing YAG transparent ceramic by double-layer embedding and sintering of zirconia and YAG powder according to claim 1 or 2, wherein the ball milling rotation speed in step (3) is 160-200 rpm, the ball milling time is 12-24 h, the drying temperature is 40-60 ℃, the drying time is 12-36 h, the sieve mesh size is 100-200 meshes, and the sieving frequency is 3-5 times.
6. The method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder according to claim 1 or 2, wherein in step (4), the dry pressing pressure is 25-35 MPa, the pressure maintaining time is 1-3 min, and the diameter of the round YAG green body is 16-30 mm; the pressure of the cold isostatic pressing is 200-240 Mpa, and the pressure maintaining time is 4-8 min.
7. The method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder according to claim 1 or 2, wherein in the step (5), the bisque firing temperature is 800-900 ℃, and the bisque firing time is 5-8 h; the degree of vacuum in the vacuum sintering furnace was 1.0X 10-5~1.0×10-3Pa, the vacuum sintering temperature is 1760-1800 ℃, and the sintering time is 8-20 h.
8. The method for preparing YAG transparent ceramic by double-layer embedding sintering of zirconia and YAG powder as claimed in claim 1 or 2, wherein the thickness ratio of the zirconia powder layer (2) to the YAG green body (4) during embedding in step (5) is 1.0-3.0, and the thickness ratio of the YAG powder layer (3) to the YAG green body (4) is 3.0-4.0.
9. The method for preparing YAG transparent ceramic by double-layer embedding and sintering of zirconia and YAG powder as claimed in claim 1 or 2, wherein the inner diameter of the tungsten crucible B (5) is 1.2-2.0 times of the outer diameter of the tungsten crucible A (1).
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