JP2002179413A - Spherical aluminum nitride filler and method of producing the same - Google Patents
Spherical aluminum nitride filler and method of producing the sameInfo
- Publication number
- JP2002179413A JP2002179413A JP2000378278A JP2000378278A JP2002179413A JP 2002179413 A JP2002179413 A JP 2002179413A JP 2000378278 A JP2000378278 A JP 2000378278A JP 2000378278 A JP2000378278 A JP 2000378278A JP 2002179413 A JP2002179413 A JP 2002179413A
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- JP
- Japan
- Prior art keywords
- aluminum nitride
- flux
- spherical
- nitride powder
- particle
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- Compounds Of Alkaline-Earth Elements, Aluminum Or Rare-Earth Metals (AREA)
- Ceramic Products (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、球状窒化アルミニ
ウムフィラー及びその製造方法に関し、主にパワーデバ
イス用の封止材用フィラーとしての用途が期待される高
熱伝導性窒化アルミニウム粉末を、樹脂に配合する際の
流動性や充填性を高める目的で球状化した球状窒化アル
ミニウム粉体とその製造方法に関するものであり、更に
詳しくは、本発明は、直接窒化法及びアルミナ還元窒化
法等により合成された不定形の窒化アルミニウム粉末を
アルカリ土類元素、希土類元素、アルミニウム、イット
リウム、リチウムの酸化物又は窒化物、乃至は加熱中の
分解により上記のものを生じる前駆体（炭酸塩、硝酸
塩、シュウ酸塩、水酸化物、ハロゲン化物、アルコキシ
ド等）よりなる単体及び複合フラックス中で熟成して球
状化した後、単離して作製した平滑な表面を持った球状
結晶質窒化アルミニウムフィラー及びその製造方法に関
する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a spherical aluminum nitride filler and a method for producing the same, which comprises mixing a high thermal conductive aluminum nitride powder, which is expected to be mainly used as a filler for an encapsulant for power devices, with a resin. The present invention relates to a spherical aluminum nitride powder that has been spheroidized for the purpose of enhancing the fluidity and filling property when performing and a method for producing the same, and more specifically, the present invention was synthesized by a direct nitriding method and an alumina reduction nitriding method. The amorphous aluminum nitride powder is converted into an alkaline earth element, a rare earth element, an oxide or nitride of aluminum, yttrium, lithium, or a precursor (carbonate, nitrate, oxalate) which is formed by decomposition during heating. , Hydroxides, halides, alkoxides, etc.) and ripened in a single or composite flux to form spheroids, then isolated Spherical crystalline aluminum nitride filler with the produced smooth surface, and a method for producing the same.
【０００２】[0002]
【従来の技術】電子部品の多くは使用中に熱を発生する
ため、その部品を適切に機能させるためには、高熱伝導
かつ電気絶縁性を有する窒化アルミニウムを放熱材料と
して利用することが期待されている。従来、封止材用窒
化アルミニウムフィラーは、主に直接窒化法により合成
した窒化アルミニウムを粉砕・分級することにより作製
されてきた。しかし、このような破砕状フィラーは、樹
脂中に配合した際の流動性に欠け、高充填化が難しかっ
た。2. Description of the Related Art Since most electronic components generate heat during use, it is expected that aluminum nitride having high thermal conductivity and electrical insulating properties will be used as a heat dissipation material in order to function properly. ing. Conventionally, an aluminum nitride filler for a sealing material has been produced mainly by pulverizing and classifying aluminum nitride synthesized by a direct nitriding method. However, such a crushed filler lacks fluidity when blended in a resin, and it is difficult to achieve high filling.
【０００３】[0003]
【発明が解決しようとする課題】このような状況の中
で、本発明者らは、樹脂に配合する際の流動性や充填性
に優れた、平滑な表面と球状の形態を持った球状結晶質
窒化アルミニウムフィラーとその製造法を開発すること
を目標として鋭意研究を重ねた結果、不定形の窒化アル
ミニウム粉体を単体又は複合フラックス中で熟成（熱処
理）して球状化する方法を採用することにより所期の目
的を達成し得ることを見出し、本発明を完成するに至っ
た。本発明の目的は、樹脂、グリース、合成ゴム等のフ
ィラーとして使用される、流動性、充填性に優れた、適
当な粒径及び粒度分布を持つ球状の窒化アルミニウム粉
体を提供することにある。Under such circumstances, the present inventors have developed a spherical crystal having a smooth surface and a spherical morphology, which is excellent in fluidity and filling property when compounded into a resin. After conducting intensive research with the aim of developing a porous aluminum nitride filler and its manufacturing method, adopting a method of aging (heat-treating) amorphous aluminum nitride powder in a simple or composite flux to make it spherical. As a result, it was found that the intended purpose could be achieved, and the present invention was completed. An object of the present invention is to provide a spherical aluminum nitride powder having an appropriate particle size and particle size distribution, which is used as a filler for resins, greases, synthetic rubbers, etc., and has excellent fluidity and filling properties. .
【０００４】[0004]
【課題を解決するための手段】上記課題を解決するため
の本発明は、以下の技術的手段から構成される。 （１）直接窒化法、アルミナ還元窒化法、気相法等によ
り合成された不定形の窒化アルミニウム粉末を、アルカ
リ土類元素、希土類元素、アルミニウム、イットリウ
ム、リチウムの酸化物又は窒化物、乃至は加熱中の分解
により上記のものを生じる炭酸塩、硝酸塩、シュウ酸
塩、水酸化物、ハロゲン化物、アルコキシド等の前駆体
よりなるフラックス中で熟成（熱処理）するか或いは、
フラックス成分を予め加えて合成された窒化アルミニウ
ム系の組成物を直接熱処理することにより、球状化させ
た後、フラックスを溶解して単離して作製した、平均粒
子径が０．１〜１００ミクロンで、平滑な表面と球状の
形態を持った、フラックス中での球状化ならびに粒成長
を特徴とする結晶質窒化アルミニウム粉体。 （２）前記（１）記載の球状窒化アルミニウム粉体を製
造する方法であって、直接窒化法、アルミナ還元窒化
法、気相法等により合成された不定形の窒化アルミニウ
ム粉末を、アルカリ土類元素、希土類元素、アルミニウ
ム、イットリウム、リチウムの酸化物又は窒化物、乃至
は加熱中の分解により上記のものを生じる炭酸塩、硝酸
塩、シュウ酸塩、水酸化物、ハロゲン化物、アルコキシ
ド等の前駆体よりなるフラックス中で熟成（熱処理）す
るか或いは、フラックス成分を予め加えて合成された窒
化アルミニウム系の組成物を直接熱処理することによ
り、球状化させた後、フラックスを溶解して単離するこ
とを特徴とする球状窒化アルミニウム粉体の製造方法。 （３）使用する不定形の窒化アルミニウム粉末の初期粒
径や粒度分布を変えて、あるいはフラックスの種類、熟
成温度、熟成時間、処理回数を変えて粒径や粒度分布を
任意に制御した前記（１）記載の球状窒化アルミニウム
粉体。 （４）前記（３）記載の粒径の異なる球状窒化アルミニ
ウム粉体を２種類以上混合して作製した充填性に優れた
球状窒化アルミニウム粉末。 （５）前記（１）、（３）又は（４）記載の球状窒化ア
ルミニウム粉末において、不定形の窒化アルミニウム原
料粉末をフラックス中で球状化した後、フラックス部分
を酸性溶液中で溶解する際に、溶液中に含まれる水によ
り窒化アルミニウム表面を部分的に酸化処理し、酸化保
護膜を付与した球状窒化アルミニウム粉体。The present invention for solving the above-mentioned problems comprises the following technical means. (1) An amorphous aluminum nitride powder synthesized by a direct nitridation method, an alumina reduction nitridation method, a gas phase method or the like is used to convert an alkaline earth element, a rare earth element, aluminum, yttrium, lithium oxide or nitride, or Ripening (heat treatment) in a flux consisting of precursors such as carbonates, nitrates, oxalates, hydroxides, halides, alkoxides, etc. which produce the above by decomposition during heating, or
An aluminum nitride-based composition synthesized by adding a flux component in advance is directly heat-treated to form a spheroid, then the flux is dissolved and isolated, and the average particle diameter is 0.1 to 100 microns. A crystalline aluminum nitride powder having a smooth surface and a spherical morphology, characterized by spheroidization and grain growth in a flux. (2) The method for producing a spherical aluminum nitride powder according to the above (1), wherein the amorphous aluminum nitride powder synthesized by a direct nitriding method, an alumina reduction nitriding method, a gas phase method or the like is used as an alkaline earth. Element, rare earth element, oxide or nitride of aluminum, yttrium, lithium, or a precursor of carbonate, nitrate, oxalate, hydroxide, halide, alkoxide, etc., which produces the above by decomposition during heating Aging (heat treatment) in a flux consisting of, or direct heat treatment of an aluminum nitride-based composition synthesized by adding a flux component in advance to form a spheroid and then dissolve and isolate the flux A method for producing a spherical aluminum nitride powder, comprising: (3) The particle size and the particle size distribution are arbitrarily controlled by changing the initial particle size and the particle size distribution of the amorphous aluminum nitride powder to be used, or by changing the type of flux, aging temperature, aging time and number of treatments. The spherical aluminum nitride powder according to 1). (4) A spherical aluminum nitride powder having excellent filling properties, prepared by mixing two or more kinds of the spherical aluminum nitride powders having different particle diameters described in the above (3). (5) In the spherical aluminum nitride powder according to the above (1), (3) or (4), after the amorphous aluminum nitride raw material powder is spheroidized in a flux, the flux portion is dissolved in an acidic solution. A spherical aluminum nitride powder obtained by partially oxidizing the surface of aluminum nitride with water contained in a solution to provide an oxidation protective film.
【０００５】[0005]
【発明の実施の形態】続いて、本発明について更に詳細
に説明する。本発明の目的は、上述のように、直接窒化
法及びアルミナ還元窒化法等により合成された不定形の
窒化アルミニウム粉末をアルカリ土類元素、希土類元
素、アルミニウム、イットリウム、リチウムの酸化物又
は窒化物、乃至は加熱中の分解により上記のものを生じ
る前駆体（炭酸塩、硝酸塩、シュウ酸塩、水酸化物、ハ
ロゲン化物、アルコキシド等）よりなる単体及び複合フ
ラックス中で熟成（熱処理）して球状化した後、酸処理
してフラックス部分を溶かし、球状粒子を単離すること
により達成された。また、原料粉末の初期粒径、熟成の
際の温度及び処理時間を調整することにより得られる球
状粒子の粒径を制御し、更に、粒径制御された数種類の
粉体を混合することにより、適当な粒度分布を持った球
状窒化アルミニウムフィラーを作製することが可能であ
る。Next, the present invention will be described in more detail. As described above, an object of the present invention is to convert an amorphous aluminum nitride powder synthesized by a direct nitriding method, an alumina reduction nitriding method, or the like into an alkaline earth element, a rare earth element, aluminum, yttrium, lithium oxide or nitride. Or aging (heat treatment) in a simple or composite flux consisting of precursors (carbonates, nitrates, oxalates, hydroxides, halides, alkoxides, etc.) which give rise to the above by decomposition during heating; This was achieved by dissolving the flux portion by acid treatment after isolation, and isolating the spherical particles. Also, the initial particle size of the raw material powder, controlling the particle size of the spherical particles obtained by adjusting the temperature and processing time during aging, further, by mixing several types of powder particle size controlled, It is possible to prepare a spherical aluminum nitride filler having an appropriate particle size distribution.
【０００６】本発明は、主にパワーデバイス用の封止材
用フィラーとしての用途が期待される高熱伝導性窒化ア
ルミニウム粉末を、樹脂に配合する際の流動性や充填性
を高める目的で球状化した窒化アルミニウム粒子とその
製造方法に関するものである。本発明においては、直接
窒化法及びアルミナ還元窒化法により合成された不定形
の窒化アルミニウム粉末をフラックス中で熟成し、球状
化させる。この場合、上記不定形の窒化アルミニウム粉
末をアルカリ土類元素、希土類元素、アルミニウム、イ
ットリウム、リチウムの酸化物又は窒化物、乃至は加熱
中の分解により上記のものを生じる前駆体（炭酸塩、硝
酸塩、シュウ酸塩、水酸化物、ハロゲン化物、アルコキ
シド等）より成るフラックスと混合するが、好適には、
上記不定形の窒化アルミニウム粉末を上記フラックスと
９５〜２０：５〜８０のモル比で混合する。次に、これ
らを熟成（熱処理）し、球状化するが、この場合、好適
には、窒素又はアルゴン雰囲気中、１６００〜２０００
℃で熱処理して得られた凝集体を、粉砕した後、塩酸、
硝酸等の適宜の酸性溶液中で攪拌しながらフラックス部
分を溶かし、平滑な表面を持った球状窒化アルミニウム
を単離する。また、上記方法と同等の方法として、上記
フラックス成分を予め加えて合成された窒化アルミニウ
ム系の組成物を直接熱処理することにより、球状化する
ことも適宜可能である。[0006] The present invention is intended to improve the fluidity and filling property of high thermal conductive aluminum nitride powder, which is expected to be mainly used as a filler for an encapsulant for power devices, when it is mixed with a resin. Aluminum nitride particles and a method for producing the same. In the present invention, an amorphous aluminum nitride powder synthesized by a direct nitriding method and an alumina reduction nitriding method is aged in a flux to be spherical. In this case, the amorphous aluminum nitride powder is converted into an alkaline earth element, a rare earth element, an oxide or nitride of aluminum, yttrium, or lithium, or a precursor (carbonate, nitrate) that is formed by decomposition during heating. , Oxalates, hydroxides, halides, alkoxides, etc.).
The amorphous aluminum nitride powder is mixed with the flux in a molar ratio of 95 to 20: 5 to 80. Next, these are aged (heat treated) and spheroidized. In this case, preferably, these are 1600 to 2000 in an atmosphere of nitrogen or argon.
Agglomerate obtained by heat treatment at ℃, crushed, hydrochloric acid,
The flux portion is dissolved while stirring in an appropriate acidic solution such as nitric acid, and spherical aluminum nitride having a smooth surface is isolated. In addition, as a method equivalent to the above method, it is possible to appropriately form a spheroid by directly heat-treating an aluminum nitride-based composition synthesized by adding the above-mentioned flux component in advance.
【０００７】上記方法において、添加したフラックス成
分（例えば、酸化カルシウム）は、窒化アルミニウム表
面の酸化アルミニウム及び一部の窒化アルミニウムと反
応して溶融物（Ｃａ−Ａｌ−Ｏ−（Ｎ）系融体）を形成
する。この溶融物中で窒化アルミニウムの溶解・析出が
起こり、窒化アルミニウムが球状化して行く。冷却後、
固化及び結晶化したフラックス部分（ＣａＡｌ2 Ｏ4 、
Ｃａ−Ａｌ−Ｏ−（Ｎ）系ガラス）は、酸に容易に溶解
し、球状窒化アルミニウムが単離される。また、本発明
において、初期粒径、熟成の際の温度、処理時間、処理
回数を調整することにより任意に粒径を制御し、更に、
粒径制御された数種類の粉体を混合することにより、適
当な粒度分布を持った高密度充填に適した球状窒化アル
ミニウムフィラーが作製できる。具体的には、例えば、
２粒径成分を混合して高密度充填を目指す場合、一般的
な粒子の充填性の向上化方法に準じて、微粒に対する粗
粒の粒径を７倍以上とし、微粒成分０．３（粗粒０．
７）程度の組成比で混合することにより充填性を高める
ことが可能である（例えば、R. K. McGreary, J. Am. C
eram. Soc., 44, 513-22 (1961) 、伊賀武雄，セラミッ
クス協会誌，１０３，８５０−５６（１９９５））。In the above method, the added flux component (for example, calcium oxide) reacts with the aluminum oxide on the surface of the aluminum nitride and a part of the aluminum nitride to form a melt (Ca-Al-O- (N) -based melt). ) Is formed. Dissolution / precipitation of aluminum nitride occurs in the melt, and the aluminum nitride becomes spherical. After cooling,
Solidified and crystallized flux portion (CaAl 2 O 4,
Ca-Al-O- (N) -based glass) is easily dissolved in an acid, and spherical aluminum nitride is isolated. Further, in the present invention, the initial particle size, the temperature at the time of ripening, the treatment time, by controlling the number of treatments arbitrarily control the particle size,
By mixing several kinds of powders with controlled particle sizes, a spherical aluminum nitride filler having an appropriate particle size distribution and suitable for high-density packing can be produced. Specifically, for example,
When two components having a particle size are mixed to achieve high-density packing, the particle size of the coarse particles is increased to 7 times or more of the fine particles according to a general method for improving the filling property of the particles, and the fine particle component is 0.3 (coarse). Grain 0.
It is possible to increase the filling property by mixing at a composition ratio of about 7) (for example, RK McGreary, J. Am. C)
eram. Soc., 44, 513-22 (1961), Takeo Iga, Journal of the Ceramic Society of Japan, 103, 850-56 (1995)).
【０００８】このようにして得られた窒化アルミニウム
は、例えば、平均粒子径が０．１〜１００ミクロンで、
平滑な表面と球状の形態を持つ。更に、数種類の粉体を
混合し、適当な粒度分布を持った球状粉末は、高い流動
性と高密度充填可能な高熱伝導性封止材等のフィラーと
して最適である。The aluminum nitride thus obtained has, for example, an average particle size of 0.1 to 100 μm,
It has a smooth surface and a spherical morphology. Further, a spherical powder having an appropriate particle size distribution obtained by mixing several kinds of powders is most suitable as a filler such as a highly heat-conductive sealing material capable of high fluidity and high-density filling.
【０００９】[0009]
【実施例】次に、実施例に基づいて本発明を具体的に説
明するが、以下の実施例は本発明の好適な一例を示すも
のであり、本発明は、当該実施例によって何ら限定され
るものではない。 実施例１ アルミナ還元窒化法により合成された窒化アルミニウム
微粉末（平均一次粒径０．５ミクロン）を炭酸カルシウ
ムと８０：２０のモル比で混合した後、窒素雰囲気中、
１７００〜１９００℃で２〜１２時間熱処理して得られ
た凝集体を、粉砕した後、（１＋１）塩酸溶液中で攪拌
しながらフラックス部分を溶かし、球状化した窒化アル
ミニウムを単離した。単離した窒化アルミニウムの平均
粒径を図１に示す。熱処理温度を１７００から１９００
℃まで、処理時間を１２時間まで延ばすことにより、平
均粒径を４ミクロンまで任意に制御することができた。
また、フラックス中での溶解再析出反応により球状化が
進むため、処理時間が長くなるほど、粒径が均一化し
た。図２に１８００℃で６時間熟成させて作製した球状
窒化アルミニウム粒子のＳＥＭ写真を示す。粒径の揃っ
た平滑な表面を持った球状窒化アルミニウム粒子である
ことが分かる。EXAMPLES Next, the present invention will be described in detail with reference to examples. The following examples show preferred examples of the present invention, and the present invention is not limited by the examples. Not something. Example 1 An aluminum nitride fine powder (average primary particle size: 0.5 μm) synthesized by an alumina reduction nitriding method was mixed with calcium carbonate at a molar ratio of 80:20, and then mixed in a nitrogen atmosphere.
The aggregate obtained by heat treatment at 1700 to 1900 ° C for 2 to 12 hours was pulverized, and then the flux portion was dissolved while stirring in a (1 + 1) hydrochloric acid solution to isolate spheroidized aluminum nitride. FIG. 1 shows the average particle size of the isolated aluminum nitride. Heat treatment temperature from 1700 to 1900
The average particle size could be arbitrarily controlled to 4 microns by extending the treatment time to 12 ° C. to 12 ° C.
In addition, since the spheroidization proceeds due to the dissolution and reprecipitation reaction in the flux, the longer the treatment time, the more uniform the particle size. FIG. 2 shows an SEM photograph of spherical aluminum nitride particles produced by aging at 1800 ° C. for 6 hours. It can be seen that the particles are spherical aluminum nitride particles having a uniform surface and a smooth surface.
【００１０】実施例２ 直接窒化法により合成された粒径の異なる３種類（ａ，
ｂ，ｃ；初期平均粒径２，７，１３ミクロン）の破砕状
窒化アルミニウム粉末を炭酸カルシウムと８０：２０の
モル比で混合した後、窒素雰囲気中、１８００℃で１２
時間熱処理して得られた凝集体を、粉砕した後、（１＋
１）塩酸溶液中で攪拌しながらフラックス部分を溶か
し、球状化した窒化アルミニウムを単離した。熟成後の
各球状窒化アルミニウムのＳＥＭ写真を図３に示す。１
８００℃、１２時間の熟成により、破砕状の角張った形
状をした粒子は、尖った部分或いは粒径の小さな粒子が
選択的に溶解し、凹んだ部分に再析出した結果、すべて
球状化された。このように初期粒径を変えることによっ
ても粒径制御が可能である。特にフィラーとして有用な
１０ミクロン以上粒径を持つ粒子についても、初期粒径
の大きな出発原料を選択することにより、比較的短時間
で作製ができる。Example 2 Three types of particles (a,
(b, c; initial average particle size of 2, 7, 13 microns) was mixed with calcium carbonate in a molar ratio of 80:20, and then mixed in a nitrogen atmosphere at 1800 ° C.
Agglomerate obtained by heat treatment for a period of time is pulverized,
1) The flux portion was dissolved while stirring in a hydrochloric acid solution, and spherical aluminum nitride was isolated. FIG. 3 shows an SEM photograph of each spherical aluminum nitride after aging. 1
As a result of aging at 800 ° C. for 12 hours, all of the crushed and angular particles were sharpened as a result of the selective dissolution of sharp or small particles and re-precipitation in the recessed portions. . Thus, the particle size can be controlled by changing the initial particle size. Particularly, particles having a particle diameter of 10 μm or more useful as a filler can be produced in a relatively short time by selecting a starting material having a large initial particle diameter.
【００１１】実施例３ アルミナ還元窒化法により合成された窒化アルミニウム
微粉末（平均一次粒径０．５ミクロン）を炭酸カルシウ
ム及び酸化イットリウム（Ｙ2 Ｏ3 ）と８０：１０：１
０、８０：２０：１０、及び８０：０：２０のモル比で
混合した後、窒素雰囲気中、１８００℃で６時間熱処理
し、球状窒化アルミニウムフィラーの作製を行った。８
０：１０：１０及び８０：２０：１０の組成比において
は、炭酸カルシウムのみをフラックスとして用いた場合
と同様に（１＋１）塩酸溶液中で攪拌しながらフラック
ス部分を溶かし、球状化した窒化アルミニウムを単離す
ることが可能であった。しかし、酸化イットリウムのみ
を使用した場合、Ｙ2 Ｏ3 やＹ4 Ａｌ2 Ｏ9 等が残留し
易い。フラックス中に析出したこれらの結晶相は、窒化
アルミニウムに比べて粒径が非常に小さいので、酸処理
後に分級処理をすることにより球状窒化アルミニウムを
単離することができる。Example 3 Aluminum nitride synthesized by the alumina reduction nitriding method
Fine powder (average primary particle size 0.5 micron)
And yttrium oxide (YTwo OThree) And 80: 10: 1
0, 80:20:10, and 80: 0: 20 molar ratio
After mixing, heat treatment at 1800 ° C for 6 hours in a nitrogen atmosphere
Then, a spherical aluminum nitride filler was produced. 8
At composition ratios of 0:10:10 and 80:20:10
Is when only calcium carbonate is used as flux
Flux while stirring in (1 + 1) hydrochloric acid solution as in
Melt the aluminum part and isolate the spherical aluminum nitride
Was possible. However, only yttrium oxide
If you useTwo OThree And YFour AlTwo O9Etc. remain
easy. These crystal phases precipitated in the flux
Acid treatment due to very small particle size compared to aluminum
After that, spherical aluminum nitride
Can be isolated.
【００１２】[0012]
【発明の効果】以上詳細に説明したように、本発明は、
直接窒化法及びアルミナ還元窒化法等により合成された
不定形の窒化アルミニウム粉末をアルカリ土類元素、希
土類元素、アルミニウム、イットリウム、リチウムの酸
化物又は窒化物、乃至は加熱中の分解により上記のもの
を生じる前駆体（炭酸塩、硝酸塩、シュウ酸塩、水酸化
物、ハロゲン化物、アルコキシド等）よりなる単体及び
複合フラックス中で熟成（熱処理）して球状化した窒化
アルミニウムとその製造方法に関するものであり、本発
明により、得られた球状窒化アルミニウムは、任意に粒
径が制御されており、更に、得られた数種類の球状粉体
を混合することにより、適当な粒度分布を持った粉末と
することが可能である。従って、この球状窒化アルミニ
ウムは、高い流動性と高密度充填性が期待でき、高熱伝
導性封止材等のフィラーとして最適である。As described in detail above, the present invention provides
Amorphous aluminum nitride powder synthesized by direct nitridation method, alumina reduction nitridation method, etc. is converted to alkaline earth element, rare earth element, aluminum, yttrium, lithium oxide or nitride, or the above by decomposition during heating Aluminum nitride nitrided and spheroidized by aging (heat treatment) in a simple or composite flux consisting of precursors (carbonates, nitrates, oxalates, hydroxides, halides, alkoxides, etc.) that form According to the present invention, the spherical aluminum nitride obtained according to the present invention has a particle diameter controlled arbitrarily, and further, by mixing several kinds of obtained spherical powders, a powder having an appropriate particle size distribution is obtained. It is possible. Therefore, this spherical aluminum nitride can be expected to have high fluidity and high-density filling property, and is most suitable as a filler such as a high thermal conductive sealing material.
【図１】単離した窒化アルミニウムの平均粒径を示す。FIG. 1 shows the average particle size of isolated aluminum nitride.
【図２】１８００℃で６時間熟成させて作製した球状窒
化アルミニウム粒子のＳＥＭ写真を示す。FIG. 2 shows an SEM photograph of spherical aluminum nitride particles produced by aging at 1800 ° C. for 6 hours.
【図３】熟成後の各球状窒化アルミニウムのＳＥＭ写真
を示す。FIG. 3 shows an SEM photograph of each spherical aluminum nitride after aging.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 川上 省二 愛知県名古屋市西区貝田町２−50 松前貝 田マンションＦ−10 (72)発明者 砥綿 篤哉 愛知県名古屋市北区八代町２−109 八代 寮304 (72)発明者 太田 一徳 愛知県尾西市北今字小家1771 (72)発明者 楠本 慶二 愛知県名古屋市名東区平和が丘３−72 ────────────────────────────────────────────────── ─── Continuing on the front page (72) Inventor Shoji Kawakami 2-50 Kaidacho, Nishi-ku, Nagoya-shi, Aichi Prefecture Matsumaegai-da Mansion F-10 (72) Inventor Totsuya Totsuya 2-, Yatsushirocho, Kita-ku, Nagoya-shi, Aichi Prefecture 109 Yatsushiro Dormitory 304 (72) Inventor Kazunori Ota 1771 Kitaimaji Oya, Onishi-shi, Aichi Prefecture (72) Inventor Keiji Kusumoto 3-72 Heiwagaoka, Meito-ku, Nagoya-shi, Aichi Prefecture
Claims (5)
法等により合成された不定形の窒化アルミニウム粉末
を、アルカリ土類元素、希土類元素、アルミニウム、イ
ットリウム、リチウムの酸化物又は窒化物、乃至は加熱
中の分解により上記のものを生じる炭酸塩、硝酸塩、シ
ュウ酸塩、水酸化物、ハロゲン化物、アルコキシド等の
前駆体よりなるフラックス中で熟成（熱処理）するか或
いは、フラックス成分を予め加えて合成された窒化アル
ミニウム系の組成物を直接熱処理することにより、球状
化させた後、フラックスを溶解して単離して作製した、
平均粒子径が０．１〜１００ミクロンで、平滑な表面と
球状の形態を持った、フラックス中での球状化ならびに
粒成長を特徴とする結晶質窒化アルミニウム粉体。1. An amorphous aluminum nitride powder synthesized by a direct nitridation method, an alumina reduction nitridation method, a gas phase method, or the like, is mixed with an alkaline earth element, a rare earth element, aluminum, yttrium, lithium oxide or nitride, Or aging (heat treatment) in a flux composed of precursors such as carbonates, nitrates, oxalates, hydroxides, halides, alkoxides, etc. which produce the above by decomposition during heating, or In addition, by directly heat-treating the synthesized aluminum nitride-based composition, after spheroidizing, the flux was dissolved and isolated to produce.
A crystalline aluminum nitride powder having an average particle diameter of 0.1 to 100 microns, having a smooth surface and a spherical morphology, characterized by spheroidization and grain growth in a flux.
体を製造する方法であって、直接窒化法、アルミナ還元
窒化法、気相法等により合成された不定形の窒化アルミ
ニウム粉末を、アルカリ土類元素、希土類元素、アルミ
ニウム、イットリウム、リチウムの酸化物又は窒化物、
乃至は加熱中の分解により上記のものを生じる炭酸塩、
硝酸塩、シュウ酸塩、水酸化物、ハロゲン化物、アルコ
キシド等の前駆体よりなるフラックス中で熟成（熱処
理）するか或いは、フラックス成分を予め加えて合成さ
れた窒化アルミニウム系の組成物を直接熱処理すること
により、球状化させた後、フラックスを溶解して単離す
ることを特徴とする球状窒化アルミニウム粉体の製造方
法。2. The method for producing a spherical aluminum nitride powder according to claim 1, wherein the amorphous aluminum nitride powder synthesized by a direct nitridation method, an alumina reduction nitridation method, a gas phase method, or the like is mixed with an alkaline earth. Group elements, rare earth elements, aluminum, yttrium, oxides or nitrides of lithium,
Or a carbonate that produces the above by decomposition during heating,
Aging (heat treatment) in a flux composed of precursors such as nitrates, oxalates, hydroxides, halides, alkoxides, or direct heat treatment of an aluminum nitride-based composition synthesized by adding a flux component in advance. A method for producing a spherical aluminum nitride powder, comprising: dissolving and isolating a flux after spheroidization.
の初期粒径や粒度分布を変えて、あるいはフラックスの
種類、熟成温度、熟成時間、処理回数を変えて粒径や粒
度分布を任意に制御した請求項１記載の球状窒化アルミ
ニウム粉体。3. The particle size and particle size distribution are controlled arbitrarily by changing the initial particle size and particle size distribution of the amorphous aluminum nitride powder to be used, or by changing the type of flux, aging temperature, aging time and number of treatments. The spherical aluminum nitride powder according to claim 1.
ルミニウム粉体を２種類以上混合して作製した充填性に
優れた球状窒化アルミニウム粉末。4. A spherical aluminum nitride powder having an excellent filling property produced by mixing two or more kinds of the spherical aluminum nitride powders having different particle diameters according to claim 3.
ミニウム粉末において、不定形の窒化アルミニウム原料
粉末をフラックス中で球状化した後、フラックス部分を
酸性溶液中で溶解する際に、溶液中に含まれる水により
窒化アルミニウム表面を部分的に酸化処理し、酸化保護
膜を付与した球状窒化アルミニウム粉体。5. The spherical aluminum nitride powder according to claim 1, wherein after the amorphous aluminum nitride raw material powder is spheroidized in a flux, the flux portion is dissolved in an acidic solution. A spherical aluminum nitride powder obtained by partially oxidizing the surface of aluminum nitride with water contained therein to provide an oxide protective film.
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