JP3175073B2 - Aluminum nitride powder - Google Patents
Aluminum nitride powderInfo
- Publication number
- JP3175073B2 JP3175073B2 JP18178894A JP18178894A JP3175073B2 JP 3175073 B2 JP3175073 B2 JP 3175073B2 JP 18178894 A JP18178894 A JP 18178894A JP 18178894 A JP18178894 A JP 18178894A JP 3175073 B2 JP3175073 B2 JP 3175073B2
- Authority
- JP
- Japan
- Prior art keywords
- aluminum nitride
- nitride powder
- oxide layer
- treatment
- aluminum
- 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.)
- Expired - Fee Related
Links
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- Compositions Of Macromolecular Compounds (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、半導体装置封止用樹脂
組成物等の複合材料に好適に使用得る新規な表面処理窒
化アルミニウムに関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a novel surface-treated aluminum nitride which can be suitably used for a composite material such as a resin composition for encapsulating a semiconductor device.
【０００２】[0002]
【従来の技術及び発明が解決しようとする課題】高発熱
性のパワートランジスタ、パワーＩＣ、高速ＬＳＩ、Ｃ
ＰＵ等の半導体素子は通常セラミックパッケージもしく
は高熱伝導性プラスチックパッケージ等により封止さ
れ、半導体装置化されている。上記セラミックパッケー
ジは、構成材料そのものが高熱伝導性、耐熱性を有し、
耐浸透性にも優れているため、温度、湿度に対して強
く、しかも中空パッケージのため機械的強度も高く信頼
性の高い封止が可能である。しかしながら、構成材料は
比較的高価なものであることと、量産性に劣る欠点があ
るため、最近では上記高熱伝導性プラスチックパッケー
ジを用いた樹脂封止が注目され、主流になりつつある。
この種の樹脂封止には、従来からエポキシ樹脂組成物が
使用されており、良好な成績を収めている。しかし、半
導体分野の技術革新によって高速化が進み、さらにパッ
ケージの小形化、薄形化が強く要求されてきており、こ
れにともなって封止材料に対して従来以上の特性（高熱
伝導性、低応力性、耐湿信頼性等）の向上が要望されて
いる。これに対応するため従来は比較的耐湿信頼性が高
く、線膨張係数が小さいと共に高熱伝導性を有するアル
ミナが充填材とし用いること等が検討されてきた。2. Description of the Related Art Highly heat-generating power transistors, power ICs, high-speed LSIs, C
A semiconductor element such as a PU is usually sealed in a ceramic package or a high thermal conductive plastic package or the like to form a semiconductor device. In the above ceramic package, the constituent materials themselves have high thermal conductivity and heat resistance,
Since it has excellent penetration resistance, it is resistant to temperature and humidity, and since it is a hollow package, it has high mechanical strength and enables highly reliable sealing. However, since the constituent materials are relatively expensive and have the disadvantage of being inferior in mass productivity, resin encapsulation using the above-described highly heat-conductive plastic package has recently attracted attention and is becoming mainstream.
Epoxy resin compositions have conventionally been used for this type of resin sealing, and have achieved good results. However, due to technological innovation in the field of semiconductors, higher speeds have been progressed, and there has been a strong demand for smaller and thinner packages. Improvements in stress properties, humidity resistance, etc.) have been demanded. To cope with this, conventionally, it has been studied to use alumina having relatively high moisture resistance reliability, a low linear expansion coefficient and high thermal conductivity as a filler.
【０００３】しかし、アルミナでは十分な熱伝導性を得
るにはかなりの高充填化をしなければならないため、流
動性等に問題があり良い成型性が得られないという欠点
がある。この問題を解決するため、近年、アルミナより
も高い熱伝導率を有する窒化アルミニウムを高熱伝導性
充填材とすることが検討されてきたが、窒化アルミニウ
ムは容易に水と反応するために著しく耐湿性が劣るとい
う欠点を持っている。この欠点を解消するために窒化ア
ルミニウム粉末の表面を溶融シリカで表面被覆すること
（特開平５−２４７１８１号）が提案されているが、十
分な耐湿性が得られない。本発明は、上記事情に鑑みな
されたもので、半導体装置封止用樹脂組成物等の複合材
料に好適に使用し得る新規な窒化アルミニウム粉末を提
供することを目的とする。なお、本発明の窒化アルミニ
ウムは、複合材料中の窒化アルミニウムの耐湿性を向上
させ、さらには窒化アルミニウム粉末表面にカーボンフ
ァンクショナル基のもつ特性を付与することができる。[0003] However, alumina has a drawback that it has to be considerably filled in order to obtain sufficient thermal conductivity, so that there is a problem in fluidity and the like and good moldability cannot be obtained. In order to solve this problem, in recent years, it has been considered to use aluminum nitride having a higher thermal conductivity than alumina as a high thermal conductive filler, but aluminum nitride easily reacts with water and thus has a remarkable moisture resistance. Has the disadvantage of being inferior. In order to solve this drawback, it has been proposed to coat the surface of aluminum nitride powder with fused silica (Japanese Patent Application Laid-Open No. 5-247181), but sufficient moisture resistance cannot be obtained. The present invention has been made in view of the above circumstances, and has as its object to provide a novel aluminum nitride powder that can be suitably used for a composite material such as a resin composition for sealing a semiconductor device. The aluminum nitride of the present invention can improve the moisture resistance of aluminum nitride in a composite material, and can impart the properties of a carbon functional group to the surface of aluminum nitride powder.
【０００４】[0004]
【課題を解決するための手段及び作用】本発明者らは、
上記目的を達成するため鋭意検討を重ねた結果、窒化ア
ルミニウム粉末の表面に酸化アルミニウム層及び酸化珪
素層を設けることにより、更には、この酸化珪素層の表
面を有機珪素化合物で処理することにより耐湿性が良好
な窒化アルミニウム粉末を得ることができることを見出
した。この窒化アルミニウム粉末は、とくに半導体封止
用樹脂組成物の充填材として非常に有用であることを知
見し、本発明をなすに至ったものである。以下、本発明
について更に詳しく説明すると本発明の窒化アルミニウ
ム粉末は窒化アルミニウム粉末の表面に酸化アルミニウ
ム層及び酸化珪素層を設けることにより、更には、この
酸化珪素層の表面を有機珪素化合物で処理することによ
り得られる新規な窒化アルミニウム粉末である。ここ
で、本発明に係わる窒化アルミニウム粉末は、例えばつ
ぎのようにして製造することができる。Means and Action for Solving the Problems The present inventors have
As a result of intensive studies to achieve the above object, as a result of providing an aluminum oxide layer and a silicon oxide layer on the surface of the aluminum nitride powder, and furthermore, treating the surface of the silicon oxide layer with an organosilicon compound to provide moisture resistance. It has been found that an aluminum nitride powder having good properties can be obtained. The present inventors have found that this aluminum nitride powder is very useful, in particular, as a filler for a resin composition for semiconductor encapsulation, and have accomplished the present invention. Hereinafter, the present invention will be described in more detail. The aluminum nitride powder of the present invention is provided with an aluminum oxide layer and a silicon oxide layer on the surface of the aluminum nitride powder, and further, the surface of the silicon oxide layer is treated with an organic silicon compound. It is a novel aluminum nitride powder obtained by this. Here, the aluminum nitride powder according to the present invention can be manufactured, for example, as follows.
【０００５】すなわち、まず、窒化アルミニウム粉末の
表面に酸化アルミニウム層を形成させるために窒化アル
ミニウム粉末の表面を酸素存在下で加熱するか又は水等
で加水分解させ乾燥させる。この時、０．５ミクロン以
上の酸化アルミニウム層を容易に形成させるためには水
等で加水分解させることが望ましい。また、酸化アルミ
ニウム層を均一に形成させるためには、水又は水とアル
コール等の溶媒中で行うことが最も好ましい。しかし、
水等の溶媒を用いると乾燥時に窒化アルミニウム粉末の
凝集が生じてしまうという問題が起こる、これを防ぐた
めには噴霧式処理乾燥装置等で処理及び乾燥させること
が好ましい。また処理温度は特に限定されないが好まし
くは２５〜１２０℃である。その後、上記の処理を施し
た窒化アルミニウム粉末の表面を、熱伝導率が高く化学
的に安定なα−アルミナ層にするために高温で処理す
る。この時の処理温度は十分なα化率を得るために１０
００℃以上が好ましい。十分な耐湿性を得るためには酸
化アルミニウム層を厚くした方が良いが、厚くしすぎる
と熱伝導性が低下してしまうため、酸化アルミニウム層
は０．５〜５ミクロンが好ましい。この窒化アルミニウ
ム粉末の表面に設けられた酸化アルミニウム層の表面に
更に酸化珪素層を設けるわけであるが、この酸化アルミ
ニウム層表面をトリアルコキシシラン又はテトラアルコ
キシシランのようなアルコキシシラン又はシリカゾル等
の酸化珪素層を形成する為の材料で処理するわけである
が、この処理については大きく分けて無溶媒系（乾式）
で行う方法と溶媒中（湿式）で行う方法が挙げられる
が、被覆処理を均一に完全に行うためには、水、アルコ
ール等の溶媒中で行うことが最も好ましい。しかし、溶
媒を用いると窒化アルミニウム粉末乾燥時に凝集が生じ
てしまい、これを用いて封止樹脂組成物を調整すると流
動性等が著しく低下するという問題が起こる。これを防
ぐためには噴霧式処理乾燥装置等で処理及び乾燥させる
ことが好ましい。また被覆処理温度は特に限定されない
が好ましくは２５〜１２０℃である。さらには被覆処理
を行う時に酢酸等の酸性触媒かジアゾビシクロウンデセ
ン等の塩基性触媒を用いることが好ましい。That is, first, in order to form an aluminum oxide layer on the surface of the aluminum nitride powder, the surface of the aluminum nitride powder is heated in the presence of oxygen or hydrolyzed with water or the like and dried. At this time, in order to easily form an aluminum oxide layer of 0.5 μm or more, it is desirable to hydrolyze with water or the like. In order to form the aluminum oxide layer uniformly, it is most preferable to carry out in water or a solvent such as water and alcohol. But,
When a solvent such as water is used, there is a problem that aluminum nitride powder is agglomerated at the time of drying. In order to prevent this, it is preferable to perform treatment and drying using a spray-type treatment dryer. The processing temperature is not particularly limited, but is preferably 25 to 120 ° C. Thereafter, the surface of the aluminum nitride powder subjected to the above treatment is treated at a high temperature in order to form a chemically stable α-alumina layer having a high thermal conductivity. At this time, the treatment temperature is set at 10 to obtain a sufficient α-rate.
It is preferably at least 00 ° C. In order to obtain sufficient moisture resistance, it is better to increase the thickness of the aluminum oxide layer. However, if the thickness is too large, the thermal conductivity decreases. Therefore, the thickness of the aluminum oxide layer is preferably 0.5 to 5 μm. A silicon oxide layer is further provided on the surface of the aluminum oxide layer provided on the surface of the aluminum nitride powder. The treatment is performed with a material for forming a silicon layer. This treatment is roughly divided into a solventless system (dry type).
And a method in a solvent (wet method). In order to uniformly and completely perform the coating treatment, it is most preferable to perform the treatment in a solvent such as water or alcohol. However, when a solvent is used, agglomeration occurs during drying of the aluminum nitride powder, and when this is used to adjust the sealing resin composition, there arises a problem that the fluidity and the like are significantly reduced. In order to prevent this, it is preferable to perform treatment and drying using a spray-type treatment drying apparatus or the like. The coating temperature is not particularly limited, but is preferably 25 to 120 ° C. Further, it is preferable to use an acidic catalyst such as acetic acid or a basic catalyst such as diazobicycloundecene when performing the coating treatment.
【０００６】その後、上記の処理を施した窒化アルミの
表面を、酸化ケイ素層にするために高温で処理する。こ
の時の処理温度は十分な酸化ケイ素化を行うために２５
０℃〜１２００℃が好ましい。より好ましくは５００℃
〜１１００℃である。有機基を有するアルコキシシラン
類又はシランカップリング剤で表面処理された窒化アル
ミニウムを高温処理する場合は、炭化ケイ素等の生成を
防ぐために徐々に温度を上げて行く方が好ましい。さら
に、十分な耐湿性を得るためには酸化ケイ素層を厚くし
た方が良いが、厚くしすぎると熱伝導性が低下してしま
うため、酸化ケイ素層は０．５〜５ミクロンが好まし
い。このようにして得られる窒化アルミニウム粉末は耐
湿に極めてすぐれているものであるが、これらの表面を
更に有機珪素化合物で処理することにより特殊な性質の
窒化アルミニウム粉末を得ることができる。これは、得
られた表面が酸化珪素層で被覆されている窒化アルミニ
ウムの表面を更に有機珪素化合物で処理するわけである
が、ここで用いられる有機ケイ素化合物とはカーボンフ
ァンクショナルシランやアルコキシ基を有するシラン類
であり、カーボンファンクショナルシランとして具体的
にはγ−グリシドキシプロピルトリメトキシシラン、γ
−グリシドキシプロピルメチルジエトキシシラン、β−
（３，４−エポキシシクロヘキシル）エチルトリメトキ
シシラン、Ｎ−β−（アミノエチル）γ−アミノプロピ
ルトリメトキシシラン、Ｎ−β−（アミノエチル）γ−
アミノプロピルメチルジエトキシシラン、γ−アミノプ
ロピルトリメトキシシラン、Ｎ−フェニル−γ−アミノ
プロピルトリメトキシシラン、γ−クロロプロピルトリ
メトキシシラン、ビニルトリエトキシシラン、トリメト
キシシリルプロピルナジック酸無水物又アルコキシ基を
有するシラン類としてはエチルトリメトキシシラン、メ
チルトリメトキシシラン、テトラメトキシシラン、テト
ラエトキシシラン、エチルトリエトキシシラン、メチル
トリエトキシシラン等が挙げられる。カーボンファンク
ショナルシランを用いた場合窒化アルミニウム粉末の表
面にそのカーボンファンクショナルの特性を付与できる
為カーボンファンクショナルシランが特に好ましい。Thereafter, the surface of the aluminum nitride that has been subjected to the above treatment is treated at a high temperature in order to form a silicon oxide layer. At this time, the treatment temperature is set at 25 to perform sufficient silicon oxide formation.
0 ° C to 1200 ° C is preferred. More preferably 500 ° C
１1100 ° C. When aluminum nitride surface-treated with an alkoxysilane having an organic group or a silane coupling agent is treated at a high temperature, it is preferable to gradually increase the temperature in order to prevent formation of silicon carbide and the like. Further, to obtain sufficient moisture resistance, it is better to increase the thickness of the silicon oxide layer. However, if the thickness is too large, the thermal conductivity is reduced. Therefore, the thickness of the silicon oxide layer is preferably 0.5 to 5 μm. The aluminum nitride powder thus obtained is extremely excellent in moisture resistance, but by treating these surfaces with an organosilicon compound, an aluminum nitride powder having special properties can be obtained. This means that the surface of the aluminum nitride whose surface is covered with a silicon oxide layer is further treated with an organosilicon compound, and the organosilicon compound used here is a carbon functional silane or an alkoxy group. Silanes having a carbon functional silane, specifically, γ-glycidoxypropyltrimethoxysilane, γ
-Glycidoxypropylmethyldiethoxysilane, β-
(3,4-epoxycyclohexyl) ethyltrimethoxysilane, N-β- (aminoethyl) γ-aminopropyltrimethoxysilane, N-β- (aminoethyl) γ-
Aminopropylmethyldiethoxysilane, γ-aminopropyltrimethoxysilane, N-phenyl-γ-aminopropyltrimethoxysilane, γ-chloropropyltrimethoxysilane, vinyltriethoxysilane, trimethoxysilylpropylnadic anhydride or alkoxy Examples of silanes having a group include ethyltrimethoxysilane, methyltrimethoxysilane, tetramethoxysilane, tetraethoxysilane, ethyltriethoxysilane, methyltriethoxysilane, and the like. When carbon functional silane is used, carbon functional silane is particularly preferable because carbon functional properties can be imparted to the surface of the aluminum nitride powder.
【０００７】有機珪素化合物の処理方法としては、窒化
アルミニウム粉末表面に酸化珪素層を形成させる時と同
様に大きく分けて無溶媒系（乾式）で行う方法と溶媒中
（湿式）で行う方法が挙げられるが、表面処理を均一に
完全に行うためには、水、アルコール等の溶媒中で行う
ことが最も好ましい。しかし、溶媒を用いると窒化アル
ミニウム粉末乾燥時に凝集が生じてしまい、これを用い
て封止樹脂組成物の充填材として使用すると流動性等が
著しく低下するという問題が起こる。これを防ぐために
は噴霧式処理乾燥装置等で処理及び乾燥させることが好
ましい。また被覆処理温度は特に限定されないが好まし
くは２５〜１２０℃である。この表面処理時に、有機珪
素化合物と加水分解触媒を併用することが好ましく、加
水分解触媒としては酢酸等の酸性触媒やアミン、ジアザ
ビシクロウンデセン等の塩基性触媒等が挙げられる。ま
た、使用される有機珪素化合物の量は全窒化アルミニウ
ム粉末重量の０．０１〜１０重量％であるが、好ましく
は０．１〜２重量％である。この加水分解処理後窒化ア
ルミニウム粉末表面に形成している酸化ケイ素層とを反
応させて強固な結合を形成させるために熱処理を行う。
処理温度は特に限定されないが５０℃以下では強固な酸
化珪素層との結合が得られず又６００℃以上では有機珪
素層が劣化されてしまう為５０〜６００℃であるがより
望ましくは８０〜２５０℃である。The method of treating an organic silicon compound is roughly divided into a method of using a solvent-free system (dry method) and a method of performing the treatment in a solvent (wet method) as in the case of forming a silicon oxide layer on the surface of aluminum nitride powder. However, in order to perform the surface treatment uniformly and completely, it is most preferable to perform the treatment in a solvent such as water or alcohol. However, when a solvent is used, agglomeration occurs during the drying of the aluminum nitride powder, and when this is used as a filler for the sealing resin composition, a problem occurs in that the fluidity and the like are significantly reduced. In order to prevent this, it is preferable to perform treatment and drying using a spray-type treatment drying apparatus or the like. The coating temperature is not particularly limited, but is preferably 25 to 120 ° C. At the time of this surface treatment, it is preferable to use an organic silicon compound and a hydrolysis catalyst in combination. Examples of the hydrolysis catalyst include an acidic catalyst such as acetic acid and a basic catalyst such as amine and diazabicycloundecene. The amount of the organosilicon compound used is 0.01 to 10% by weight, preferably 0.1 to 2% by weight, based on the total weight of the aluminum nitride powder. After this hydrolysis treatment, heat treatment is performed to react with the silicon oxide layer formed on the surface of the aluminum nitride powder to form a strong bond.
The treatment temperature is not particularly limited, but if it is 50 ° C. or less, a strong bond with the silicon oxide layer is not obtained, and if it is 600 ° C. or more, the organic silicon layer is deteriorated. ° C.
【０００８】[0008]
【発明の効果】本発明の窒化アルミニウム粉末は、耐湿
性にすぐれさらには窒化アルミニウム粉末表面にカーボ
ンファンクショナルの特性を自由に付与できる為複合材
料の充填材として好適であり、特に半導体封止用樹脂組
成物の充填材として好適に使用される。The aluminum nitride powder of the present invention is excellent as a filler for a composite material because it has excellent moisture resistance and can freely impart carbon functional properties to the surface of the aluminum nitride powder. It is suitably used as a filler for a resin composition.
【０００９】[0009]
【実施例】以下、実施例を示し、本発明を具体的に説明
するが、本発明は下記の実施例に制限されるものではな
い。 ［実施例１］純水１ｋｇと平均粒径約２５ミクロンの窒
化アルミ粉末１ｋｇをガラス容器中で８０℃、４時間撹
はんした後、噴霧式処理乾燥装置で１５０℃の雰囲気中
において乾燥させ、更に１２００℃で３時間処理し、酸
化アルミニウム層を有する窒化アルミニウム粉末〔Ｉ〕
を得た。次に、噴霧式処理乾燥装置を用いて、５０℃の
雰囲気中においてメチルトリメトキシシラン２０ｇと水
８ｇ、酢酸０．８ｇ、メタノール２０ｇの混合溶液を上
記窒化アルミニウム粉末〔Ｉ〕１ｋｇに噴霧し、その後
雰囲気温度を１５０℃に上昇させ、粉末を乾燥させ更に
この粉末を１５０℃で２時間、さらに５００℃で３時間
加熱し、最後に１０００℃で３時間処理し、表面に酸化
珪素層を有する窒化アルミニウム粉末〔II〕１ｋｇを得
た。さらに、上記の噴霧式処理乾燥装置で５０℃の雰囲
気中において、この粉末〔II〕１ｋｇにメチルトリメト
キシシラン１０ｇと水５ｇ、酢酸０．５ｇ、メタノール
１０ｇの混合溶液を噴霧し、その後雰囲気温度を１５０
℃に上昇させ、粉末を乾燥させ、新規表面処理窒化アル
ミニウム〔III 〕１ｋｇを得た。The present invention will be described below in more detail with reference to Examples, but the present invention is not limited to the following Examples. [Example 1] 1 kg of pure water and 1 kg of aluminum nitride powder having an average particle size of about 25 microns were stirred in a glass container at 80 ° C for 4 hours, and then dried in an atmosphere of 150 ° C by a spray-type drying apparatus. And further treated at 1200 ° C. for 3 hours to obtain an aluminum nitride powder having an aluminum oxide layer [I]
I got Next, using a spray-type treatment drying apparatus, a mixed solution of 20 g of methyltrimethoxysilane, 8 g of water, 0.8 g of acetic acid, and 20 g of methanol was sprayed on 1 kg of the aluminum nitride powder [I] in an atmosphere of 50 ° C. Thereafter, the atmosphere temperature is raised to 150 ° C., the powder is dried, and the powder is heated at 150 ° C. for 2 hours, further heated at 500 ° C. for 3 hours, and finally treated at 1000 ° C. for 3 hours, and has a silicon oxide layer on the surface. 1 kg of aluminum nitride powder [II] was obtained. Further, a mixed solution of 10 g of methyltrimethoxysilane, 5 g of water, 0.5 g of acetic acid, and 10 g of methanol was sprayed on 1 kg of the powder [II] in an atmosphere of 50 ° C. using the above-mentioned spray treatment drying apparatus. To 150
C., and the powder was dried to obtain 1 kg of a new surface-treated aluminum nitride [III].
【００１０】［実施例２］実施例１において製造した表
面に酸化珪素層を有する窒化アルミニウム粉末〔II〕を
用いメチルトリメトキシシラン１０ｇの代りにγ−アミ
ノプロピルトリエトキシシラン１０ｇを用いほかは実施
例１と全く同様にして窒化アルミニウム粉末〔IV〕を得
た。Example 2 The same procedure as in Example 1 was repeated except that aluminum nitride powder [II] having a silicon oxide layer on the surface was used, and 10 g of γ-aminopropyltriethoxysilane was used instead of 10 g of methyltrimethoxysilane. An aluminum nitride powder [IV] was obtained in exactly the same manner as in Example 1.
【００１１】［実施例３］実施例１において製造した表
面に酸化アルミニウム層を有する窒化アルミニウム粉末
〔Ｉ〕を用い、メチルトリメトキシシラン２０ｇの代り
にビニルトリメトキシシラン２０ｇ及びメチルトリメト
キシシラン１０ｇの代りにγ−グリシドキシプロピルト
リメトキシシラン１０ｇを用いる他は実施例１と全く同
様にし窒化アルミニウム粉末〔Ｖ〕を得た。Example 3 Using aluminum nitride powder [I] having an aluminum oxide layer on the surface produced in Example 1, 20 g of vinyltrimethoxysilane and 10 g of methyltrimethoxysilane were used instead of 20 g of methyltrimethoxysilane. An aluminum nitride powder [V] was obtained in exactly the same manner as in Example 1 except that 10 g of γ-glycidoxypropyltrimethoxysilane was used instead.
【００１２】［実施例４］噴霧式処理乾燥装置を用いて
５０℃の雰囲気中においてメチルトリメトキシシラン１
０ｇと水５ｇ、酢酸０．５ｇ、メタノール１０ｇの混合
溶液を平均粒径２５ミクロンの窒化アルミ粉末１ｋｇに
噴霧し、その後雰囲気温度を１５０℃に上昇させて粉末
を乾燥させ、窒化アルミ粉末〔VI〕１ｋｇを得た。この
粉末を１５０℃で２時間加熱し、さらに５００℃で３時
間加熱し、最後に１０００℃で３時間処理し、酸化ケイ
素層を有する窒化アルミニウム粉末〔VII〕１ｋｇを得
た。Example 4 Methyltrimethoxysilane 1 in an atmosphere of 50 ° C. using a spray-type treatment drying apparatus
A mixed solution of 0 g, 5 g of water, 0.5 g of acetic acid, and 10 g of methanol was sprayed on 1 kg of aluminum nitride powder having an average particle size of 25 μm, and then the atmosphere temperature was raised to 150 ° C. to dry the powder. 1 kg was obtained. This powder was heated at 150 ° C. for 2 hours, further heated at 500 ° C. for 3 hours, and finally treated at 1000 ° C. for 3 hours to obtain 1 kg of aluminum nitride powder [VII] having a silicon oxide layer.
【００１３】［実施例５］実施例４においてメチルトリ
メトキシシラン１０ｇの代りにγ−グリシドキシプロピ
ルシラン１０ｇ、γ−アミノプロピルトリエトキシシラ
ン１０ｇを用い他は実施例４と全く同様にしそれぞれ窒
化アルミニウム粉末〔VIII〕及び〔IX〕を得た。Example 5 In Example 4, γ-glycidoxypropylsilane 10 g and γ-aminopropyltriethoxysilane 10 g were used in place of methyltrimethoxysilane 10 g. Aluminum powders [VIII] and [IX] were obtained.
【００１４】［実施例６］実施例１〜５でそれぞれ得ら
れた窒化アルミニウム粉末〔Ｉ〕〜〔IX〕８００重量部
と、樹脂成分としてＹＸ４０００（油化シェルエポキシ
（株）社製）４５重量部、ＸＬ−２２５（三井東圧化学
工業（株）社製）４８重量部、ブロム化エポキシ樹脂
（ＡＥＲ−７５５旭チバ（株）社製）７重量部、さらに
硬化促進剤としてテトラフェニルホスホニウムテトラフ
ェニルボレート３重量部、離型剤としてカルナバワック
ス１．２重量部、添加剤としてγ−グリシドキシプロピ
ルトリメトキシシラン２．０重量部、三酸化アンチモン
８重量部を混合し、ロール混練り機を用いて溶融混練し
て目的の組成物を製造した。Example 6 800 parts by weight of the aluminum nitride powders [I] to [IX] obtained in Examples 1 to 5 and 45 parts by weight of YX4000 (manufactured by Yuka Shell Epoxy Co., Ltd.) as a resin component Parts, XL-225 (manufactured by Mitsui Toatsu Chemicals, Inc.), 48 parts by weight, brominated epoxy resin (AER-755, manufactured by Asahi Ciba Co., Ltd.), 7 parts by weight, and tetraphenylphosphonium tetra as a curing accelerator 3 parts by weight of phenyl borate, 1.2 parts by weight of carnauba wax as a release agent, 2.0 parts by weight of γ-glycidoxypropyltrimethoxysilane as an additive, and 8 parts by weight of antimony trioxide were mixed, and a roll kneader was used. To obtain a target composition.
【００１５】これらの封止樹脂組成物を用いて、熱伝導
率耐湿性の試験を行った。その結果を表に示す。 「熱伝導率」それぞれの組成物を１７５℃、７０ｋｇ／
ｃｍ2 、成形時間２分の条件でトランスファー成形した
後１８０℃で４時間後硬化させ得られた５０ｍｍφ×６
ｍｍの試験片を上部ヒーターと熱量計及び下部ヒーター
の間にサンドイッチ状に挿入し、空気圧にて一定に密着
させ、５０℃で定常状態に達した後の試験片両面間の温
度差、熱量計出力から自動的に熱コンダクタンスを算出
し、この熱コンダクタンスの値と試験片の厚さとの積か
ら熱伝導率を求めた。 「耐湿性」それぞれの組成物を用いて２本のアルミニウ
ム配線を有する半導体チップを、１７５℃、７０ｋｇ／
ｃｍ2 、成形時間２分の条件でトランスファー成形した
後１８０℃で４時間後硬化させた。この半導体装置１０
０個について１２０℃の高圧水蒸気中で耐湿試験を行
い、アルミニウム腐食による５０％断線不良発生の起こ
る時間を測定した。Using these sealing resin compositions, a heat conductivity / moisture resistance test was conducted. The results are shown in the table. "Thermal conductivity" Each composition was heated at 175 ° C and 70 kg /
After transfer molding under the conditions of cm 2 and molding time of 2 minutes, 50 mmφ × 6 obtained by post-curing at 180 ° C. for 4 hours.
mm test piece is inserted between the upper heater and the calorimeter and the lower heater in a sandwich manner, and closely adhered by air pressure. After reaching a steady state at 50 ° C., the temperature difference between both surfaces of the test piece, calorimeter The thermal conductance was automatically calculated from the output, and the thermal conductivity was determined from the product of the value of the thermal conductance and the thickness of the test piece. "Moisture resistance" A semiconductor chip having two aluminum wirings was prepared by using each composition at 175 ° C and 70 kg /
After transfer molding under the conditions of cm 2 and molding time of 2 minutes, post-curing was performed at 180 ° C. for 4 hours. This semiconductor device 10
A moisture resistance test was performed on the 0 pieces in high-pressure steam at 120 ° C., and the time when 50% disconnection failure occurred due to aluminum corrosion was measured.
【００１６】 [0016]
【００１７】以上の結果で理解されるよう本発明の窒化
アルミニウム粉末〔II〕〜〔Ｖ〕は、〔Ｉ〕，〔VI〕〜
〔IX〕に比べて、熱伝導性、耐湿性にすぐれたエポキシ
樹脂組成物を得ることができる。As can be understood from the above results, the aluminum nitride powders [II] to [V] of the present invention have the following properties: [I], [VI] to
An epoxy resin composition having excellent heat conductivity and moisture resistance can be obtained as compared with [IX].
───────────────────────────────────────────────────── フロントページの続き (56)参考文献 特開 平７−315813（ＪＰ，Ａ) 特開 平４−93362（ＪＰ，Ａ) 特開 平４−268324（ＪＰ，Ａ) 特開 平６−144808（ＪＰ，Ａ) (58)調査した分野(Int.Cl.7，ＤＢ名) C01B 21/072 ＣＡ（ＳＴＮ)──────────────────────────────────────────────────続 き Continuation of the front page (56) References JP-A-7-315813 (JP, A) JP-A-4-93362 (JP, A) JP-A-4-268324 (JP, A) 144808 (JP, A) (58) Field surveyed (Int. Cl. 7 , DB name) C01B 21/072 CA (STN)
Claims (4)
ミニウム層及び酸化珪素層が設けられた窒化アルミニウ
ム粉末。1. An aluminum nitride powder in which an aluminum oxide layer and a silicon oxide layer are provided on the surface of the aluminum nitride powder.
ミニウム層及び酸化珪素層が設けられた窒化アルミニウ
ム粉末の表面が有機珪素化合物で表面処理された窒化ア
ルミニウム粉末。2. An aluminum nitride powder in which an aluminum oxide layer and a silicon oxide layer are provided on the surface of the aluminum nitride powder, and the surface of the aluminum nitride powder is surface-treated with an organosilicon compound.
ものである請求項２の窒化アルミニウム粉末。3. The aluminum nitride powder according to claim 2, wherein the organosilicon compound has an alkoxy group.
ナルシランである請求項２の窒化アルミニウム粉末。4. The aluminum nitride powder according to claim 2, wherein the organosilicon compound is carbon functional silane.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP18178894A JP3175073B2 (en) | 1994-07-11 | 1994-07-11 | Aluminum nitride powder |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP18178894A JP3175073B2 (en) | 1994-07-11 | 1994-07-11 | Aluminum nitride powder |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH0826707A JPH0826707A (en) | 1996-01-30 |
| JP3175073B2 true JP3175073B2 (en) | 2001-06-11 |
Family
ID=16106890
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP18178894A Expired - Fee Related JP3175073B2 (en) | 1994-07-11 | 1994-07-11 | Aluminum nitride powder |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3175073B2 (en) |
Families Citing this family (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2006036931A (en) * | 2004-07-27 | 2006-02-09 | Three M Innovative Properties Co | Heat-conductive composition |
| JP4907998B2 (en) * | 2006-01-18 | 2012-04-04 | 住友大阪セメント株式会社 | Resin composition |
| JP5351426B2 (en) * | 2008-03-27 | 2013-11-27 | タマティーエルオー株式会社 | Processing method of aluminum nitride powder |
| CN106750546B (en) * | 2010-02-18 | 2022-06-17 | 昭和电工材料株式会社 | Composite particle and method for producing same, resin composition, metal foil with resin, and resin sheet |
| JP5392178B2 (en) * | 2010-05-13 | 2014-01-22 | 日立化成株式会社 | High thermal conductive composite particles and heat dissipation material using the same |
| WO2012098735A1 (en) * | 2011-01-19 | 2012-07-26 | 日立化成工業株式会社 | Liquid crystal resin composition, heat dissipation material precursor, and heat dissipation material |
| CN105308121B (en) * | 2013-06-25 | 2018-09-18 | 味之素株式会社 | Resin combination |
| WO2018037913A1 (en) * | 2016-08-22 | 2018-03-01 | 富士フイルム株式会社 | Light-shielding composition, light-shielding film, solid imaging element, color filter, and liquid-crystal display device |
| JPWO2019244531A1 (en) * | 2018-06-21 | 2021-07-08 | 株式会社Adeka | Manufacturing method of surface-treated aluminum nitride, surface-treated aluminum nitride, resin composition, and cured product |
-
1994
- 1994-07-11 JP JP18178894A patent/JP3175073B2/en not_active Expired - Fee Related
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| Publication number | Publication date |
|---|---|
| JPH0826707A (en) | 1996-01-30 |
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