JP4458409B2 - Method for producing translucent ceramics and translucent ceramics - Google Patents
Method for producing translucent ceramics and translucent ceramics Download PDFInfo
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本発明は、高圧ナトリウムランプ発光管、高温炉の窓、赤外線検出用窓材、耐熱性レンズ等のように、高温下（特に、１０００℃以上）での耐久性と、紫外・可視・赤外領域波長の光に対する高い透光性とを必要とする部品の材料として好適な、透光性酸窒化アルミニウムマグネシウム焼結体に関するものである。 In the present invention, durability such as high pressure sodium lamp arc tube, high-temperature furnace window, infrared detection window material, heat-resistant lens, etc., durability at high temperatures (particularly 1000 ° C. or higher), ultraviolet / visible / infrared The present invention relates to a translucent aluminum magnesium oxynitride sintered body that is suitable as a material for parts that require high translucency with respect to light of a region wavelength.
近年、可視および赤外領域波長の光の透光性に優れ、かつ耐熱性や耐摩耗性にも優れた透光性材料に対する要求が高まっている。アルミナに窒化アルミニウムを添加し、高温で焼結すると単一相の酸窒化アルミニウムが得られることが知られている（特許文献１、２、非特許文献１）。酸窒化アルミニウムの結晶構造は、等方性の立方晶構造からなるものであり、この酸窒化アルミニウムを用いると、結晶粒界における複屈折による光散乱がなく、透光性の非常に高い酸窒化アルミニウム焼結体が得られる可能性がある。
これまで、上記酸窒化アルミニウムの均一な焼結体の製造方法として、一旦、酸窒化アルミニウム組成とした原料粉末を製造し、これを窒素中や真空中でホットプレスすることによって、透光性酸窒化アルミニウム焼結体を製造する方法が提案されている。しかし、この方法では、製造工程が複雑であり、高コストである。 Up to now, as a method for producing a uniform sintered body of aluminum oxynitride, a raw material powder once having an aluminum oxynitride composition is produced, and this is hot-pressed in nitrogen or in vacuum, thereby translucent acid. A method for producing an aluminum nitride sintered body has been proposed. However, in this method, the manufacturing process is complicated and expensive.
本発明の課題は、酸窒化アルミニウム相を主成分とする透光性の高い透光性セラミックスを常圧焼結によって得られるようにすることである。 An object of the present invention is to obtain a translucent ceramic having a high translucency mainly composed of an aluminum oxynitride phase by atmospheric pressure sintering.
本発明は、Ａｌ２Ｏ３およびＡｌＮをモル比率で８０〜６０％：２０〜４０％の割合で含有し、かつ平均粒径０．６〜１．２μｍのＭｇＯ粉末をＡｌ２Ｏ３とＡｌＮとの合計量を１００重量部としたときに２〜１０重量部含有する混合粉末を成形して成形体を得、この成形体を最高温度１９５０〜２０５０℃で焼結させ、前記最高温度への昇温時に１５００〜１７５０℃の温度で保持し、少なくとも１７００℃から前記最高温度までの昇温速度を０．５〜８℃／分とすることを特徴とする、ＡｌＯＮ相を主相とする透光性セラミックスの製造方法に係るものである。
The present invention contains Al 2 O 3 and AlN at a molar ratio of 80 to 60%: 20 to 40%, and MgO powder having an average particle size of 0.6 to 1.2 μm is mixed with Al 2 O 3 and AlN. molding a mixed powder containing 2 to 10 parts by weight when the total amount was 100 parts by weight of the obtained molded body, and sintered the molded body at a maximum temperature of 1950-2050 ° C., to the maximum temperature It is maintained at a temperature of 1500 to 1750 ° C. at the time of temperature increase, and the rate of temperature increase from at least 1700 ° C. to the maximum temperature is 0.5 to 8 ° C./min. The present invention relates to a method for producing a photoceramic.
この方法によれば、酸窒化アルミニウム相を主成分とする透光性の高い透光性セラミックスを常圧焼結によって得ることができる。
透光性セラミックスのうち最も量の多い相はＡｌＯＮ相である必要がある。好ましくはＸ線回折測定において、ＡｌＯＮ相のピーク強度と他の結晶相のピーク強度との合計値を１００％としたとき、他の結晶相のピーク強度は１０％以下であることが好ましく、５％以下であることが更に好ましい。
According to this method, a translucent ceramic having a high translucency mainly composed of an aluminum oxynitride phase can be obtained by atmospheric pressure sintering.
Of translucent ceramics, the most abundant phase needs to be an AlON phase. Preferably, in the X-ray diffraction measurement, when the total value of the peak intensity of the AlON phase and the peak intensity of the other crystal phase is 100%, the peak intensity of the other crystal phase is preferably 10% or less. % Or less is more preferable.
Ａｌ２Ｏ３およびＡｌＮの割合は、モル比率で８０〜６０％：２０〜４０％の割合とする。これによって酸窒化アルミニウム相を主相として生成させることができる。Ａｌ２Ｏ３とＡｌＮとの合計量を１００重量部としたときにＭｇＯ粉末を２〜１０重量部添加する。ＭｇＯ粉末の添加量を２重量部以上とすることによって、結晶粒子径を大きくすることができ、直線透過率が向上する。この観点からは、ＭｇＯ粉末の添加量を２重量部以上とすることが好ましい。また、ＭｇＯ粉末の添加量が１０重量部を超えると、焼結時の粒内気孔が多く存在し透光性が劣る。
The proportions of Al 2 O 3 and AlN are 80 to 60% and 20 to 40% in terms of molar ratio. Thereby, an aluminum oxynitride phase can be generated as a main phase. When the total amount of Al 2 O 3 and AlN is 100 parts by weight, 2 to 10 parts by weight of MgO powder is added. By making the addition amount of
ＭｇＯ粉末の平均粒径は０．６〜１．２μｍとする。例えば非特許文献１においてはＭｇＯ粉末の平均粒径は０．４μｍと微細であるが、焼結温度によって直線透過率の変化が非常に大きく、焼結温度による特性変動が大きい。本発明のように若干平均粒径の大きいＭｇＯ粉末を使用することで、最終的な焼結体中にＡｌ２Ｏ３相が残り易くなり、焼結温度による直線透過率の変化が小さく、従って安定して高い直線透過率を有する焼結体を量産可能となる。 The average particle diameter of MgO powder shall be 0.6-1.2 micrometers. For example, in Non-Patent Document 1, the average particle diameter of MgO powder is as fine as 0.4 μm, but the change in linear transmittance is very large depending on the sintering temperature, and the characteristic variation due to the sintering temperature is large. By using MgO powder having a slightly larger average particle diameter as in the present invention, the Al 2 O 3 phase tends to remain in the final sintered body, and the change in linear transmittance due to the sintering temperature is small. A sintered body having a stable and high linear transmittance can be mass-produced.
成形体の焼結時の最高温度は１９５０〜２０５０℃とする。この最高温度を１９５０℃以上、２０５０℃以下とすることによって、焼結体の直線透過率を高くすることができる。 The maximum temperature during sintering of the molded body is 1950-2050 ° C. By setting the maximum temperature to 1950 ° C. or more and 2050 ° C. or less, the linear transmittance of the sintered body can be increased.
本発明においては、常圧焼結で少なくとも１７００℃から最高温度までの昇温速度を０．５〜８℃／分とする。このように固相反応から燒結までの昇温速度を低くし、反応を緩やかにすることによって、急激な緻密化を抑えながら、粒内気孔を拡散し、結晶粒子を成長させて透光性を高くすることができる。この観点からは、１７００℃以上での昇温速度を２℃／分以下とすることが更に好ましい。
In the present invention, the rate of temperature increase from at least 1700 ° C. to the maximum temperature is 0.5-8 ° C./min in normal pressure sintering. In this way, by lowering the rate of temperature rise from the solid-phase reaction to sintering and slowing the reaction, while suppressing rapid densification, it diffuses intra-granular pores and grows crystal grains to increase translucency. Can be high. From this viewpoint, it is more preferable to set the rate of temperature rise at 1700 ° C. or higher to 2 ° C./min or lower.
また、本発明は、前記方法によって得られたことを特徴とする透光性セラミックスに係るものである。この透光性セラミックスは、好ましくはＡｌ２Ｏ３相を含有している。特に好ましくは、ＡｌＯＮ相とＡｌ２Ｏ３相との各ピーク高さの相対比率が、実施例記載の条件で９５．０〜９９．５：５．０〜０．５である。 The present invention also relates to a translucent ceramic obtained by the above method. This translucent ceramic preferably contains an Al 2 O 3 phase. Particularly preferably, the relative ratio of the peak heights of the AlON phase and the Al 2 O 3 phase is 95.0 to 99.5: 5.0 to 0.5 under the conditions described in the examples.
以下本発明に係る透光性酸窒化アルミニウムマグネシウム焼結体の製造方法について、さらに詳細に説明する。まず、アルミナ粉末、窒化アルミニウム粉末および酸化マグネシウム粉末を所定の配合比で混合して混合粉末を調製する。アルミナ粉末の平均粒径は０．４μｍ以下であることが好ましく、窒化アルミニウム粉末の平均粒径は０．６μｍ以下であることが好ましい。酸化マグネシウム粉末の平均粒径は０．６μｍ以上、１．２μｍ以下とする。 Hereinafter, the manufacturing method of the translucent aluminum magnesium oxynitride sintered compact concerning this invention is demonstrated in detail. First, a mixed powder is prepared by mixing alumina powder, aluminum nitride powder and magnesium oxide powder at a predetermined blending ratio. The average particle size of the alumina powder is preferably 0.4 μm or less, and the average particle size of the aluminum nitride powder is preferably 0.6 μm or less. The average particle diameter of the magnesium oxide powder is 0.6 μm or more and 1.2 μm or less.
粉末混合方法は限定されない。例えば、エタノール等の溶媒中で各粉末をボールミル中で混合し、得られたスラリーをスプレードライなどの方法によって乾燥して調製することによって、混合状態の良い混合粉末が得られる。 The powder mixing method is not limited. For example, each powder is mixed in a ball mill in a solvent such as ethanol, and the obtained slurry is dried and prepared by a method such as spray drying, whereby a mixed powder having a good mixing state can be obtained.
次に、上記混合粉末を成形し、成形体を得る。この成形方法は限定されない。例えば、金型を用いた一軸加圧成形、ゴム型を用いた冷間等方加圧（ＣＩＰ）成形を例示できる。上記のようにボールミルを用いて混合した場合には、前記スラリーを、石膏などの多孔質の型に直接に流し込み、混合粉末を型に着肉した後、離型および乾燥することによって、成形体を得ることができる。 Next, the mixed powder is molded to obtain a molded body. This forming method is not limited. For example, uniaxial pressure molding using a mold and cold isostatic pressing (CIP) molding using a rubber mold can be exemplified. When mixed using a ball mill as described above, the slurry is poured directly into a porous mold such as gypsum, and after the mixed powder is placed in the mold, the molded product is released and dried. Can be obtained.
そして、成形体を大気圧あるいは減圧下で所定の最高温度まで昇温させることによって、固相反応および焼結を行わせる。この際、最高温度までゆっくりと昇温することによって、固相反応を生じさせ、次いで焼結を生じさせることができる。最高温度よりも低い温度において一定時間保持することによって、アルミナ粉末、窒化アルミニウム粉末および酸化マグネシウム粉末の固相反応を進行させ、酸窒化アルミニウムマグネシウム（Ｍｇ−Ａｌ−Ｏ−Ｎ）相を生成させることができる。この後に保持温度から最高温度へと昇温し、焼結を生じさせる。
Then, the molded body is heated to a predetermined maximum temperature under atmospheric pressure or reduced pressure to cause solid phase reaction and sintering. At this time, by slowly raising the temperature to the maximum temperature, a solid phase reaction can be caused, and then sintering can be caused. By maintaining the temperature at a temperature lower than the maximum temperature for a certain period of time, the solid phase reaction of the alumina powder, the aluminum nitride powder and the magnesium oxide powder proceeds to produce an aluminum magnesium oxynitride (Mg—Al—O—N) phase. Can do. Thereafter, the temperature is raised from the holding temperature to the maximum temperature to cause sintering.
前記保持温度は、１５００〜１７５０℃の温度範囲が好適である。上記保持温度が１７５０℃を超えると、以降の処理で除去できない閉気孔が焼結体中に残留しやすく、最終製品の透光性を下げるおそれがある。 The holding temperature is preferably in a temperature range of 1500 to 1750 ° C. When the holding temperature exceeds 1750 ° C., closed pores that cannot be removed by the subsequent treatment are likely to remain in the sintered body, which may reduce the translucency of the final product.
固相反応および焼結時の雰囲気ガスには、窒素ガス、水素ガス、又はアルゴンなどの不活性ガスを用いることができる。また、焼結中の成形体の還元を防ぐために、上記窒素ガス等や不活性ガス中に０．１〜５％程度の酸素ガスを混合したガスを用いてもよい。 An inert gas such as nitrogen gas, hydrogen gas, or argon can be used as the atmospheric gas during the solid phase reaction and sintering. Moreover, in order to prevent the reduction | restoration of the molded object during sintering, you may use the gas which mixed about 0.1-5% oxygen gas in the said nitrogen gas etc. or inert gas.
成形体の固相反応が進行すると、更に最高温度へと昇温し、焼結体とする。最高温度での保持時間は３〜１０時間が適当である。 When the solid-phase reaction of the molded body proceeds, the temperature is further raised to the maximum temperature to obtain a sintered body. The holding time at the maximum temperature is suitably 3 to 10 hours.
以下のようにして、表１のＴー１〜１３に示す各例の焼結体を作製した。
（粉末） 具体的には、Ａｌ２Ｏ３粉末（住友化学株式会社製「ＡＫＰ−３０」：平均粒径０．４μｍ、ＡｌＮ粉末（徳山ソーダ株式会社製「ＦグレードＡｌＮ粉末」：平均粒径０．６μｍ）、およびＭｇＯ粉末（宇部マテリアルズ株式会社製「高純度超微紛」：平均粒径１．０μｍ）を使用した。
The sintered body of each example shown to T-1-13 of Table 1 was produced as follows.
(Powder) Specifically, Al 2 O 3 powder (“AKP-30” manufactured by Sumitomo Chemical Co., Ltd .: average particle size 0.4 μm, AlN powder (“F grade AlN powder” manufactured by Tokuyama Soda Co., Ltd.): average particle size 0.6 μm), and MgO powder (“Upure Materials Co., Ltd.“ High-purity ultrafine powder ”: average particle size 1.0 μm) were used.
（調合条件） １リットルポリ容器内に径φ５ｍｍのアルミナ玉石１ｋｇ（純度99.9％）、前記原料粉末およびエタノール(500cc)を加え、ポットミル中で２４時間混合・解砕し（70〜80rpm），調合物を得た。各粉末の混合比率は、表１に示すように変更した。
（溶媒除去・乾燥）
ステンレスバットに調合物を収容し、N２ガス乾燥機内で、１０５０℃で１２時間乾燥した。
（粉砕・篩通し）
乾燥後の調合物を、純度９９．９％アルミナ乳鉢を用いて粉砕し、ポリエステル篩（＃８０）に通した。
（ペレット成形）
ハンドプレスφ20金型に調合物を収容し、圧力200kg／ｃｍ２で成形し、ペレット状の成形体を得た。このペレット状成形体を、ＣＩＰで2000ｋｇ／ｃｍ２で加圧した。
（焼成）
図１に模式的に示すようなカーボン製の匣鉢１を準備した。３は匣鉢本体であり、２は蓋である。匣鉢１の寸法は、縦３００ｍｍ、横３００ｍｍ、高さ２００ｍｍである。匣鉢１内に窒化ホウ素製のルツボ５を収容した。図２に模式的に示すように、ルツボ５の本体７の空間８内に窒化ホウ素粉末９を充填し、窒化ホウ素粉末９内にペレット状成形体１０を埋設する。そして窒化ホウ素製の蓋６をする。ルツボの寸法は、直径８０ｍｍ、高さ７０ｍｍである。
（研磨）
各例の焼結体を、厚さ１．２ｍｍになるまで研磨加工し、次いで焼結体の両面を鏡面研磨加工した。
(Mixing conditions) Add 1 kg of alumina cobblestone (purity 99.9%) with a diameter of 5 mm in a 1 liter plastic container, the raw material powder and ethanol (500 cc), mix and disintegrate in a pot mill for 24 hours (70-80 rpm), and mix I got a thing. The mixing ratio of each powder was changed as shown in Table 1.
(Solvent removal / drying)
The preparation was placed in a stainless steel vat and dried at 1050 ° C. for 12 hours in an N 2 gas dryer.
(Crushing and sieving)
The dried formulation was pulverized using an alumina mortar with a purity of 99.9% and passed through a polyester sieve (# 80).
(Pellet molding)
The preparation was housed in a hand press φ20 mold and molded at a pressure of 200 kg / cm 2 to obtain a pellet-shaped molded body. The pellet-like molded body was pressurized with CIP at 2000 kg / cm 2 .
(Baking)
A carbon bowl 1 as schematically shown in FIG. 1 was prepared. 3 is a mortar body, and 2 is a lid. The dimensions of the mortar 1 are 300 mm in length, 300 mm in width, and 200 mm in height. A
(Polishing)
The sintered body of each example was polished until the thickness became 1.2 mm, and then both surfaces of the sintered body were mirror-polished.
表１に示す各例においては、以下のような昇温−焼成−降温スケジュールを採用した。
（Ｔ−１、Ｔ−２）
室温から２０００℃まで１０℃／分で昇温し、２０００℃で１０時間保持した。予備加熱工程は設けていない。
（Ｔ−３、Ｔ−４）
室温から保持温度１７５０℃まで１０℃／分で昇温し、１７５０℃で３時間保持し、更に最高温度２０５０℃まで１０℃／分で昇温した。そして２０５０℃で６時間保持した。
（Ｔ−５、６、７、８）
室温から保持温度１７００℃まで１０℃／分で昇温し、１７００℃で１時間保持し、更に最高温度２０００℃まで２℃／分で昇温した。そして２０００℃１０時間保持した。
（Ｔ−９、１０、１１、１１）
室温から保持温度１７００℃まで１０℃／分で昇温し、１７００℃で１時間保持し、更に最高温度２０５０℃まで２℃／分で昇温した。そして２０５０℃３時間保持した。
（Ｔ−１３）
室温から保持温度１７００℃まで１０℃／分で昇温し、１７００℃で１時間保持し、更に最高温度２０５０℃まで１．３℃／分で昇温した。そして２０５０℃で３時間保持した。
In each example shown in Table 1, the following temperature increase-firing-temperature decrease schedule was adopted.
(T-1, T-2)
The temperature was raised from room temperature to 2000 ° C. at a rate of 10 ° C./min, and kept at 2000 ° C. for 10 hours. There is no preheating step.
(T-3, T-4)
The temperature was raised from room temperature to a holding temperature of 1750 ° C. at 10 ° C./min, held at 1750 ° C. for 3 hours, and further raised to a maximum temperature of 2050 ° C. at 10 ° C./min. And it hold | maintained at 2050 degreeC for 6 hours.
(T-5, 6, 7, 8)
The temperature was raised from room temperature to a holding temperature of 1700 ° C. at 10 ° C./min, held at 1700 ° C. for 1 hour, and further raised to a maximum temperature of 2000 ° C. at 2 ° C./min. And it hold | maintained at 2000 degreeC for 10 hours.
(T-9, 10, 11, 11)
The temperature was raised from room temperature to a holding temperature of 1700 ° C. at 10 ° C./min, held at 1700 ° C. for 1 hour, and further raised to a maximum temperature of 2050 ° C. at 2 ° C./min. And it hold | maintained at 2050 degreeC for 3 hours.
(T-13)
The temperature was raised from room temperature to a holding temperature of 1700 ° C. at 10 ° C./min, held at 1700 ° C. for 1 hour, and further raised to a maximum temperature of 2050 ° C. at 1.3 ° C./min. And it hold | maintained at 2050 degreeC for 3 hours.
得られた各例の焼結体について、以下の特性を測定した。
（生成相）
以下の条件で各焼結体のＸ線回折チャートを得た。
CuKα、50kV、300mA 、2 θ＝１０〜７０°
回転対陰極型X 線回折装置「理学電機製「RINT」」
この結果、いずれの例においても、ＡｌＯＮ相とＡｌ２Ｏ３相との各ピークを検出した。更に、各ピークの高さを合計し、ピーク高さの合計値を１００％とした。そしてＡｌＯＮ相、Ａｌ２Ｏ３相の各ピーク高さ比率（％）を測定した。
（粒径）
焼結した試料断面をＳＥＭで粒径サイズを観察した。
（密度、相対密度）
アルキメデス法によって測定した。
（直線透過率）
焼成した試料を１３ｍｍ×１３ｍｍ×１．２ｍｍｔの寸法に加工し、試料両面をダイヤモンドペーストで鏡面研磨した試料を，直線透過率測定器で波長６００ｎｍの透過率を測定した。
The following characteristics were measured for the obtained sintered bodies of the respective examples.
(Generation phase)
An X-ray diffraction chart of each sintered body was obtained under the following conditions.
CuKα, 50kV, 300mA, 2θ = 10-70 °
Rotating anti-cathode X-ray diffractometer "RINT" manufactured by Rigaku Corporation
As a result, in each example, each peak of the AlON phase and the Al2O3 phase was detected. Furthermore, the height of each peak was totaled and the total value of the peak height was set to 100%. And each peak height ratio (%) of the AlON phase and the Al 2 O 3 phase was measured.
(Particle size)
The particle size of the sintered sample cross section was observed by SEM.
(Density, relative density)
Measured by Archimedes method.
(Linear transmittance)
The fired sample was processed into a size of 13 mm × 13 mm × 1.2 mmt, and the sample whose both surfaces were mirror-polished with diamond paste was measured for transmittance at a wavelength of 600 nm with a linear transmittance meter.
比較例のＴ−１においては、ＭｇＯを添加しておらず、２０００℃まで１０℃／分で昇温し、２０００℃で焼結させている。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３（Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は２％であった。試料の直線透過率は１％と低かった。本発明外のＴ−２においては、ＭｇＯを３．０重量％添加し、Ｔ−１と同じ焼成条件を採用している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３ （Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は１．７％であった。相対密度は９６．０％と若干低く、試料の直線透過率は２１％に達していた。
In T-1 of the comparative example, MgO is not added, the temperature is increased to 2000 ° C. at 10 ° C./min, and sintering is performed at 2000 ° C. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 2%. The linear transmittance of the sample was as low as 1%. In T-2 outside the present invention, MgO is added in an amount of 3.0% by weight, and the same firing conditions as T-1 are employed. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 1.7%. The relative density was slightly low as 96.0%, and the linear transmittance of the sample reached 21%.
比較例のＴ−３においては、ＭｇＯを添加しておらず、１７５０℃で３時間保持しており，また２０５０℃まで１０℃／分で昇温している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３（Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は２％であった。試料の直線透過率は１％と低かった。本発明外のＴ−４においては、ＭｇＯを３．０重量％添加し、Ｔ−３と同じ条件で焼結している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３ （Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は１．５％であった。相対密度は９６．４％と若干低く、試料の直線透過率は９％であった。
In T-3 of the comparative example, MgO was not added, the temperature was maintained at 1750 ° C. for 3 hours, and the temperature was increased to 2050 ° C. at 10 ° C./min. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 2%. The linear transmittance of the sample was as low as 1%. In T-4 outside the present invention, 3.0 wt% of MgO is added and sintered under the same conditions as T-3. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 1.5%. The relative density was slightly low as 96.4%, and the linear transmittance of the sample was 9%.
本発明例のＴ−５においては、ＭｇＯを３．０重量％添加しており、１７００℃で１時間保持しており，また２０００℃まで２℃／分で昇温している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３（Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は４．３％であった。試料の相対密度は９８．５％と高く、試料の直線透過率は４１％と高かった。比較例のＴ−６、７、８においては、ＭｇＯを添加しておらず、Ｔ−５と同じ条件で焼結している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３ （Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は２．５％であった。試料の相対密度は高いが、比較例の試料Ｔ−１、３とほとんど変わらない。これに対して、ＭｇＯ粉末を添加している本発明例Ｔ−２、４、５においては、最高温度への昇温速度が試料の相対密度に対して大きく影響しており、この点で比較例とまったく異なっている。比較例Ｔ−６、７、８の直線透過率は、それぞれ、５、２、２％であった。 In T-5 of the example of the present invention, 3.0 wt% of MgO is added, held at 1700 ° C. for 1 hour, and heated up to 2000 ° C. at 2 ° C./min. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 4.3%. The relative density of the sample was as high as 98.5%, and the linear transmittance of the sample was as high as 41%. In Comparative Examples T-6, 7, and 8, MgO was not added, and sintering was performed under the same conditions as T-5. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 2.5%. Although the relative density of the sample is high, it is almost the same as the samples T-1 and 3 of the comparative example. On the other hand, in the present invention examples T-2, 4 and 5 in which MgO powder is added, the temperature increase rate to the maximum temperature has a great influence on the relative density of the sample. It is completely different from the example. The linear transmittances of Comparative Examples T-6, 7, and 8 were 5, 2, and 2%, respectively.
本発明例のＴ−９においては、ＭｇＯを３．０重量％添加しており、１７００℃で１時間保持しており，また２０５０℃まで２℃／分で昇温している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３（Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は４．３％であった。試料の相対密度は９９．２％と高く、試料の直線透過率は４３％と高かった。比較例のＴ−１０、１１、１２においては、ＭｇＯを添加しておらず、Ｔ−９と同じ条件で焼結している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３ （Ｃｏｒｕｄｕｍ）が残存している複合相であった。試料の相対密度は高いが、比較例の試料Ｔ−１、３、６、７、８とほとんど変わらない。比較例Ｔ−１０、１１、１２の直線透過率は、それぞれ、５、３、３％であった。比較例の試料Ｔ−１０、Ｔ−１１、Ｔ−１２において、Ａｌ２O３相のピーク高さ比率は４．３％、２．５％、２．５％であった。
更に、ＭｇＯを３重量％添加したＴ−９では試料の粒径が大きく、ＭｇO無添加のＴ−１０、１１、１２では試料の粒径は約１／５まで小さくなった。
In T-9 of the present invention example, 3.0% by weight of MgO was added, held at 1700 ° C. for 1 hour, and increased to 2050 ° C. at 2 ° C./min. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 4.3%. The relative density of the sample was as high as 99.2%, and the linear transmittance of the sample was as high as 43%. In Comparative Examples T-10, 11, and 12, MgO was not added, and sintering was performed under the same conditions as T-9. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. Although the relative density of the sample is high, it is almost the same as the samples T-1, 3, 6, 7, and 8 of the comparative example. The linear transmittances of Comparative Examples T-10, 11, and 12 were 5, 3, and 3%, respectively. In Comparative Samples T-10, T-11, and T-12, the Al 2 O 3 phase peak height ratios were 4.3%, 2.5%, and 2.5%.
Furthermore, the particle size of the sample was large in T-9 to which 3% by weight of MgO was added, and the particle size of the sample was reduced to about 1/5 in T-10, 11 and 12 to which MgO was not added.
本発明例のＴ−１３においては、ＭｇＯを３．０重量％添加しており、１７００℃で１時間保持しており，また２０５０℃まで１．３℃／分で昇温している。得られた焼結体のＸ線回折分析を行うと、ＡｌＯＮ単相の結晶が得られず、僅かにＡｌ２O３（Ｃｏｒｕｄｕｍ）が残存している複合相であった。Ａｌ２O３相のピーク高さ比率は４．１％であった。試料の直線透過率は３１％と高かった。 In T-13 of the present invention example, 3.0% by weight of MgO was added, held at 1700 ° C. for 1 hour, and increased to 2050 ° C. at 1.3 ° C./min. When the X-ray diffraction analysis of the obtained sintered body was performed, AlON single-phase crystals were not obtained, and it was a composite phase in which Al 2 O 3 (Corudum) remained slightly. The peak height ratio of the Al 2 O 3 phase was 4.1%. The linear transmittance of the sample was as high as 31%.
以上述べたように、本発明によれば、酸窒化アルミニウム相を主成分とする透光性の高い透光性セラミックスを常圧焼結によって得ることができる。 As described above, according to the present invention, a highly transparent translucent ceramic mainly composed of an aluminum oxynitride phase can be obtained by atmospheric pressure sintering.
１ 匣鉢 ２ 蓋 ３ 匣鉢本体 ５ ルツボ ７ ルツボ本体 ９ 窒化ホウ素粉末 １０ 成形体
DESCRIPTION OF SYMBOLS 1
Claims (4)
The relative proportion of each peak heights of the AlON phase and the Al 2 O 3 phase is 95.0 to 99.5: characterized in that it is a 5.0 to 0.5, according to claim 3, wherein the translucent ceramics .
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