JPH02153995A - Silicone grease composition - Google Patents

Silicone grease composition

Info

Publication number
JPH02153995A
JPH02153995A JP30751388A JP30751388A JPH02153995A JP H02153995 A JPH02153995 A JP H02153995A JP 30751388 A JP30751388 A JP 30751388A JP 30751388 A JP30751388 A JP 30751388A JP H02153995 A JPH02153995 A JP H02153995A
Authority
JP
Japan
Prior art keywords
aluminum nitride
thermal conductivity
silicone grease
grease composition
examples
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.)
Granted
Application number
JP30751388A
Other languages
Japanese (ja)
Other versions
JPH0639591B2 (en
Inventor
Takayuki Takahashi
孝行 高橋
Satoshi Kuwata
桑田 敏
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Shin Etsu Chemical Co Ltd
Original Assignee
Shin Etsu Chemical Co Ltd
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Shin Etsu Chemical Co Ltd filed Critical Shin Etsu Chemical Co Ltd
Priority to JP63307513A priority Critical patent/JPH0639591B2/en
Publication of JPH02153995A publication Critical patent/JPH02153995A/en
Publication of JPH0639591B2 publication Critical patent/JPH0639591B2/en
Anticipated expiration legal-status Critical
Expired - Fee Related legal-status Critical Current

Links

Abstract

PURPOSE:To obtain the subject composition for heat dissipation having low oil repellency and especially excellent in thermo-conductivity by blending an organopolysiloxane with powdery aluminum nitride of spherical hexagonal system in a specified ratio. CONSTITUTION:The objective composition is composed of (A) 100 pts. wt. organopolysiloxane represented by the formula [R is 1-18C (preferably 6-14C) monovalent hydrocarbon; a is 1.8-2.3] and (B) 100-900 pts. wt. powdery aluminum nitride of spherical hexagonal system with 0.5-5mum average particle size. In addition viscosity of the component (A) is required to be 50-500,000cs, especially preferably 100-100,000cs at 25 deg.C.

Description

【発明の詳細な説明】 (産業上の利用分野) 本発明はシリコーングリース組成物に関し、特に熱伝導
性に優れた放熱用シリコーングリース組成物に関する。
DETAILED DESCRIPTION OF THE INVENTION (Industrial Application Field) The present invention relates to a silicone grease composition, and particularly to a heat dissipating silicone grease composition with excellent thermal conductivity.

(従来の技術) 従来から、シリコーンオイルをベースとした放熱用グリ
ースとして亜鉛華やアルミナ粉末を増稠剤として使用し
たものが知られている(特公昭52−33272、特公
昭59−52195)、又、近年、更に熱伝導率の向上
を達成し得る増稠剤として窒化アルミニウムが開発され
ている(例えば特公昭60−14792及び特公昭57
−36302)。
(Prior Art) Conventionally, silicone oil-based heat dissipation greases using zinc white or alumina powder as thickeners have been known (Japanese Patent Publications No. 52-33272, No. 59-52195). In addition, in recent years, aluminum nitride has been developed as a thickener that can further improve thermal conductivity (for example, Japanese Patent Publication No. 60-14792 and Japanese Patent Publication No. 14792).
-36302).

(発明が解決しようとする課題) しかしながら、窒化アルミニウムのオイル保持力が十分
でないために、従来においてはシリコーンオイル中に含
有せしめることのできる窒化アルミニウムの量は極めて
限られており、従って、窒化アルミニウム自身の熱伝導
性は良いものの、シリコーングリース組成物としての熱
伝導性についてはあまり改善がなされていない。例えば
特公昭60−14792号公報に記載された発明におい
ては、シリコーンオイル100重量部に対して、窒化ア
ルミニウム粉末を50〜95重量部添加するが、これで
は添加量が少な(十分な熱伝導率の向上を期待すること
ができない。
(Problem to be Solved by the Invention) However, because the oil retention power of aluminum nitride is not sufficient, the amount of aluminum nitride that can be contained in silicone oil is extremely limited in the past. Although silicone grease itself has good thermal conductivity, little improvement has been made in the thermal conductivity of silicone grease compositions. For example, in the invention described in Japanese Patent Publication No. 60-14792, 50 to 95 parts by weight of aluminum nitride powder is added to 100 parts by weight of silicone oil, but this amount is too small (sufficient thermal conductivity cannot be expected to improve.

又、特公昭57−36302号公報に記載された発明に
おいては、薄片状窒化アルミニウム粉末が任意成分とな
っているが、オイル保持力を向上させる目的で球状シリ
カファイバーを必須成分としているために、窒化アルミ
ニウム粉末の含有量が低下せざるを得す、やはり十分な
熱伝導率の向上を期待することはできない。
Furthermore, in the invention described in Japanese Patent Publication No. 57-36302, flaky aluminum nitride powder is an optional component, but spherical silica fiber is an essential component for the purpose of improving oil retention. The content of aluminum nitride powder has to be reduced, and a sufficient improvement in thermal conductivity cannot be expected.

本発明者等は、従来のかかる欠点を解決すべく鋭意研究
の結果、特定のオルガノポリシロキサンと一定粒径範囲
の球状六方晶系窒化アルミニウム粉末とを組み合わせる
ことにより、シリコーンオイル中に極めて多量の窒化ア
ルミニウムを含有せしめることができることを見い出し
本発明に到達した。
As a result of intensive research to solve these conventional drawbacks, the present inventors have discovered that by combining a specific organopolysiloxane and spherical hexagonal aluminum nitride powder with a certain particle size range, an extremely large amount of silicone oil can be contained. The present invention was achieved by discovering that aluminum nitride can be contained.

従って本発明の目的は、離油度が小さく、熱伝導性の良
好なシリコーングリース組成物を提供することにある。
Therefore, an object of the present invention is to provide a silicone grease composition that has a low degree of oil separation and good thermal conductivity.

(課題を解決するための手段) 本発明の上記の諸口的は一般式Ra5IO,i、−で表
されるオルガノポリシロキサン100重量部と、平均粒
径が0.5〜5μmであって球状六方晶系の窒化アルミ
ニウム粉末100〜900重量部とから成るシリコーン
グリース組成物によって達成された。
(Means for Solving the Problems) The above aspects of the present invention include 100 parts by weight of an organopolysiloxane represented by the general formula Ra5IO,i, This was achieved with a silicone grease composition comprising 100 to 900 parts by weight of crystalline aluminum nitride powder.

本発明における第一成分としてのオルガノポリシロキサ
ンは、Ra5iO5,において、Rは炭素数1〜18よ
り成る、飽和又は不飽和の一価の炭化水素基の群から選
択される一種若しくは二種以上の基である。このような
基としては、例えばメチル基、エチル基、プロピル基、
ヘキシル基、オクチル基、デシル基、ドデシル基、テト
ラデシル基、ヘキサデシル基、オクタデシル基などの飽
和炭化水素& 、ビニール基、フェニル基、クロロフェ
ニル基などの不飽和炭化水素基等が挙げられるが、特に
メチル基、フェニル基及び炭素数6〜14のアルキル基
等が好ましい。
The organopolysiloxane as the first component in the present invention is Ra5iO5, where R is one or more selected from the group of saturated or unsaturated monovalent hydrocarbon groups having 1 to 18 carbon atoms. It is the basis. Examples of such groups include methyl, ethyl, propyl,
Examples include saturated hydrocarbon groups such as hexyl, octyl, decyl, dodecyl, tetradecyl, hexadecyl, and octadecyl groups, and unsaturated hydrocarbon groups such as vinyl, phenyl, and chlorophenyl groups, but especially methyl A phenyl group, an alkyl group having 6 to 14 carbon atoms, and the like are preferred.

又、aは1.8〜2.3である。Further, a is 1.8 to 2.3.

本発明で使用するオルガノポリシロキサンの粘度は、゛
−シリコーングリース組成物として要求される稠度及び
熱伝導性の観点から25°Cで、50〜500.000
csであることが必要であり、特に100〜100.0
00csであることが好ましい。
The viscosity of the organopolysiloxane used in the present invention is 50 to 500,000 at 25°C from the viewpoint of consistency and thermal conductivity required for a silicone grease composition.
cs, especially 100 to 100.0
It is preferable that it is 00cs.

本発明においては、シリコーングリース組成物に熱伝導
性を付与する窒化アルミニウム粉末として、特にオイル
保持力に優れた球状六方晶系窒化アルミニウム粉末を第
二成分として使用する。この場合上記窒化アルミニウム
粉末の平均粒径を0゜5μm以下とすると、増稠効果が
大きすぎて稠度の低い(硬い)グリースとなり、使用上
好ましいグリースが得られない、従って、平均粒径が0
゜5μm以下の球状六方晶系粉末を用いて使用上好まし
いグリースとするためには、窒化アルミニウム粉末の含
有量を少なくせねばならず、少なくすれば、当然のこと
ながら本来の目的である熱伝導性が乏しいものとなるの
で好ましくない。又、平均粒径が5μmよりも大きい場
合には、でき上がったグリースの均一性が乏しく、グリ
ースとしての安定性が悪い上離油度が大きくベースオイ
ルの分離も激しいものとなるので好ましくない、従って
本発明においては、使用する球状六方晶系の平均粒径を
0.5〜5μmとすることが必要である。
In the present invention, as the aluminum nitride powder that imparts thermal conductivity to the silicone grease composition, a spherical hexagonal aluminum nitride powder particularly excellent in oil retention is used as the second component. In this case, if the average particle size of the aluminum nitride powder is 0.5 μm or less, the thickening effect will be too large and the consistency will be low (hard), making it difficult to obtain a grease that is suitable for use.
In order to make a grease that is suitable for use using spherical hexagonal powder with a diameter of 5 μm or less, the content of aluminum nitride powder must be reduced. This is not desirable because it results in poor quality. In addition, if the average particle size is larger than 5 μm, the finished grease will have poor uniformity and stability as a grease, and the degree of oil separation will be large and the separation of the base oil will be severe, which is undesirable. In the invention, it is necessary that the average particle diameter of the spherical hexagonal system used be 0.5 to 5 μm.

本発明のグリースを製造するには、前記第−成分及び第
二成分を計量し、プラネタリ−ミキサー等の混合機にて
混合する。又、必要に応じて酸化防止剤等の公知の第三
成分を添加しても良い。混合は、例えば加圧下又は減圧
下で加熱混合を行ったのち、三本ロールなどの混練り機
で十分に混練りすることによって行うことができる。
To produce the grease of the present invention, the first component and second component are weighed and mixed using a mixer such as a planetary mixer. Further, a known third component such as an antioxidant may be added as necessary. Mixing can be carried out, for example, by heating and mixing under pressure or reduced pressure, and then sufficiently kneading with a kneader such as a three-roll kneader.

上記の如くして製造した本発明のグリースの離油度(J
 I S−に−2220による)は、120’C/24
時間の条件で0〜0.8%と非常に少く、また、真空理
工■製TCW−1,000型熱線法熱伝導率計によれば
、従来のグリースの熱伝導率が1.0〜2. OX 1
0−”c a l/crs−s e c″Cであるのに
対して、本発明のグリースの場合には2、 5〜5. 
5 X 10−’c a 17cm−s e c’cと
、大巾にその熱伝導性を改良することができる。
Oil separation degree (J
IS-2220) is 120'C/24
According to the TCW-1,000 type hot wire method thermal conductivity meter manufactured by Shinku Riko ■, the thermal conductivity of conventional grease is 1.0 to 2. .. OX1
0-"cal/crs-sec"C, whereas in the case of the grease of the present invention, it is 2.5-5.
5 x 10-'ca 17 cm-sec'c, the thermal conductivity can be greatly improved.

(発明の効果) 以上の如くして得られた本発明のシリコーングリース組
成物は、離油度が小さくオイル分Mmが少ない上、熱伝
導性も良好であり、従来の熱伝導性グリースよりもはる
かに優れた性能を有する。
(Effects of the Invention) The silicone grease composition of the present invention obtained as described above has a low oil separation degree and a low oil content Mm, and also has good thermal conductivity, which is better than conventional thermally conductive greases. Has much better performance.

(実施例) 以下、本発明を実施例によって更に詳述するが、本発明
はこれによって限定されるものではない。
(Examples) Hereinafter, the present invention will be explained in more detail with reference to Examples, but the present invention is not limited thereto.

実施例1〜9゜ 表1に示す粘度を有する、後記各種のオルガノポリシロ
キサン100重量部をベースオイルとし、このベースオ
イルに、同表に示す平均粒径を有する球状六方晶系窒化
アルミニウム粉末を同表に示す量、計量して添加し、プ
ラネタリ−ミキサーで30分間両者を十分に混合した後
、三本ロールによる混練りを3回実施して本発明のシリ
コーング表−1 尚、表1で使用したベースオイルは夫々下記のものであ
る。
Examples 1 to 9 100 parts by weight of various organopolysiloxanes listed below having the viscosity shown in Table 1 were used as a base oil, and spherical hexagonal aluminum nitride powder having the average particle size shown in the same table was added to the base oil. The amount shown in Table 1 was measured and added, and the two were sufficiently mixed for 30 minutes using a planetary mixer, and then kneaded three times using three rolls to obtain the silicone compound of the present invention. The base oils used are as follows.

実施例1〜4:両末端トリメチルシリル基封鎖ジメチル
ポリシロキサン 実施例5〜78両末端トリメチルシリル基封鎖ジメチル
デシルメチルポリシロキ サン(デシル基25モル%) 実施例8〜9:両末端トリメチルシリル基封鎖ジメチル
ジフェニルポリシロキ サン(フェニル基25モル%) 得られた何れの試料も、外観は淡灰色で滑らかな表面を
しており均一なグリース状であった。又、120℃、2
4時間後の離油度は低く、極めて良好であった。
Examples 1 to 4: Dimethylpolysiloxane blocked with trimethylsilyl groups at both ends Examples 5 to 78 Dimethyldecylmethylpolysiloxane blocked with trimethylsilyl groups at both ends (25 mol % of decyl groups) Examples 8 to 9: Dimethyldiphenyl polysiloxane blocked at both ends with trimethylsilyl groups Siloxane (25 mol % of phenyl groups) All the samples obtained had a light gray appearance, a smooth surface, and a uniform grease-like appearance. Also, 120℃, 2
The degree of oil separation after 4 hours was low and extremely good.

各試料について真空理工■製TCW−1,000型熱伝
導率測定装W(熱線法)を用いて夫々の熱伝導率を測定
した結果は表−2に示した通りである。
The thermal conductivity of each sample was measured using a TCW-1,000 model thermal conductivity measuring instrument W (hot wire method) manufactured by Shinku Riko ■, and the results are shown in Table 2.

表−2の結果は、本発明のシリコーングリース組成物の
熱伝導率が、後記比較例で代表される従来からのグリー
スに比べ、格段に優れていることを実証している。
The results in Table 2 demonstrate that the thermal conductivity of the silicone grease composition of the present invention is significantly superior to that of conventional greases typified by Comparative Examples below.

表−2 尚、表中の稠度及び離油度の測定はJIS−に−222
0によって行った。
Table 2 The consistency and oil separation in the table are measured according to JIS-222.
It was done by 0.

比較例1〜6゜ 表−3に示す如く、ベースオイルと増稠剤を用いて実施
例の場合と同様にして試料を作製した。
Comparative Examples 1 to 6 As shown in Table 3, samples were prepared in the same manner as in the examples using base oil and a thickener.

表−3 得られた各試料について夫々、稠度、離油度及び熱伝導
率を実施例の場合と同様に測定した。
Table 3 For each sample obtained, the consistency, oil separation degree, and thermal conductivity were measured in the same manner as in Examples.

比較例NO,1のグリースは、滑らかさは良好であるが
、窒化アルミニウム粉末の添加量が少ないため十分な熱
伝導率が得られなかった。
Although the grease of Comparative Example No. 1 had good smoothness, sufficient thermal conductivity could not be obtained because the amount of aluminum nitride powder added was small.

比較例No、2のグリースは硬くなりすぎ、伸展性に乏
しく使用に耐えられないものとなった。
The greases of Comparative Examples No. 2 and 2 were too hard and had poor extensibility, making them unusable.

比較例N003のグリースは、熱伝導率は良好な値を示
したがグリースとしての均一性に欠け、放置後のオイル
分離が激しいものとなった。
The grease of Comparative Example No. 003 showed a good thermal conductivity value, but lacked uniformity as a grease, and oil separation after standing was severe.

比較例No、4及び5のグリースは従来からの亜鉛華粉
末を使用したものであるが、何れの場合も、グリースの
均一性は優れているものの熱伝導率は低いものであった
The greases of Comparative Examples Nos. 4 and 5 used conventional zinc white powder, and in all cases, although the uniformity of the grease was excellent, the thermal conductivity was low.

比較例N006のグリースは、アルミナ粉末を使用した
ものであるが、熱伝導率は亜鉛華の場合と同程度の低い
ものであり、比較的オイル分離量の多いものであった。
Although the grease of Comparative Example No. 006 used alumina powder, its thermal conductivity was as low as that of zinc white, and the amount of oil separated was relatively large.

これらの結果をまとめると表−4に示す如くであり、何
れの試料の性能も実施例によって得られた本願発明のシ
リコーングリース組成物の性能より格段に劣ることが確
認された。
These results are summarized as shown in Table 4, and it was confirmed that the performance of each sample was significantly inferior to the performance of the silicone grease composition of the present invention obtained in the Examples.

尚、使用したベースオイルは、比較例1及び2の場合に
は共に両末端トリメチルシリル基封鎖ジメチルポリシロ
キサン、比較例3及び4の場合には、両末端トリメチル
シリル基封饋ジメチルデシルメチルポリシロキサン(デ
シル基25モル%)、比較例5及び6の場合には、両末
端トリメチルシリル基封鎖ジメチルジフェニルポリシロ
キサン(フェニル基25モル%)である。
The base oil used was dimethylpolysiloxane with trimethylsilyl groups capped at both ends in Comparative Examples 1 and 2, and dimethyldecylmethylpolysiloxane with trimethylsilyl groups capped at both ends in Comparative Examples 3 and 4. In the case of Comparative Examples 5 and 6, it was dimethyldiphenylpolysiloxane (25 mol% of phenyl groups) blocked at both ends with trimethylsilyl groups.

以上の実施例、比較例の結果は、本発明の熱放射用シリ
コーングリース組成物の性能が、従来品に比して格段に
優れていることを実証するものである。
The results of the above Examples and Comparative Examples demonstrate that the performance of the heat radiation silicone grease composition of the present invention is significantly superior to conventional products.

特許出願人 信越化学工業株式会社 代 理 人Patent applicant: Shin-Etsu Chemical Co., Ltd. teenager Reason Man

Claims (1)

【特許請求の範囲】[Claims] 一般式RaSiO_4_−_a_/_2で表されるオル
ガノポリシロキサン100重量部と、平均粒径が0.5
〜5μmであって球状六方晶系の窒化アルミニウム粉末
100〜900重量部とから成るシリコーングリース組
成物;一般式中、Rは炭素数1〜18の飽和又は不飽和
の一価の炭化水素基の群から選択される一種若しくは二
種以上の基であり、aは1.8〜2.3である。
100 parts by weight of organopolysiloxane represented by the general formula RaSiO_4_-_a_/_2 and an average particle size of 0.5
A silicone grease composition comprising 100 to 900 parts by weight of spherical hexagonal aluminum nitride powder with a diameter of 5 μm; in the general formula, R represents a saturated or unsaturated monovalent hydrocarbon group having 1 to 18 carbon atoms; is one or more groups selected from the group, and a is 1.8 to 2.3.
JP63307513A 1988-12-05 1988-12-05 Silicone grease composition Expired - Fee Related JPH0639591B2 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP63307513A JPH0639591B2 (en) 1988-12-05 1988-12-05 Silicone grease composition

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP63307513A JPH0639591B2 (en) 1988-12-05 1988-12-05 Silicone grease composition

Publications (2)

Publication Number Publication Date
JPH02153995A true JPH02153995A (en) 1990-06-13
JPH0639591B2 JPH0639591B2 (en) 1994-05-25

Family

ID=17969982

Family Applications (1)

Application Number Title Priority Date Filing Date
JP63307513A Expired - Fee Related JPH0639591B2 (en) 1988-12-05 1988-12-05 Silicone grease composition

Country Status (1)

Country Link
JP (1) JPH0639591B2 (en)

Cited By (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0896031A3 (en) * 1997-08-06 2000-01-26 Shin-Etsu Chemical Co., Ltd. Thermally conductive silicone composition
JP2000169873A (en) * 1998-12-02 2000-06-20 Shin Etsu Chem Co Ltd Silicone grease composition
US6136758A (en) * 1998-08-17 2000-10-24 Shin-Etsu Chemical Co., Ltd. Aluminum nitride powder and thermally conductive grease composition using the same
US6632780B2 (en) 2001-01-04 2003-10-14 Hitachi, Ltd. Highly thermal conductive grease composition and cooling device using the same
EP1378542A1 (en) * 2001-03-09 2004-01-07 Dow Corning Toray Silicone Co., Ltd. Greasy silicone composition
US7510998B2 (en) 2004-05-21 2009-03-31 Shin-Etsu Chemical Co., Ltd. Silicon grease compositions
US8017684B2 (en) 2005-12-27 2011-09-13 Shin-Etsu Chemical Co., Ltd. Heat conductive silicone grease compositions
JP6068733B2 (en) * 2014-08-26 2017-01-25 バンドー化学株式会社 Thermally conductive resin molded product
EP3150672A1 (en) 2015-10-02 2017-04-05 Shin-Etsu Chemical Co., Ltd. Thermal conductive silicone composition and semiconductor device
WO2019093052A1 (en) 2017-11-09 2019-05-16 信越化学工業株式会社 Thermally conductive silicone grease composition
KR20190077345A (en) 2016-10-31 2019-07-03 신에쓰 가가꾸 고교 가부시끼가이샤 Thermally conductive silicone composition, semiconductor device and method of manufacturing semiconductor device
EP3575363A1 (en) 2018-05-31 2019-12-04 Shin-Etsu Chemical Co., Ltd. Low heat resistance silicone composition
WO2020129555A1 (en) 2018-12-21 2020-06-25 信越化学工業株式会社 Heat-conductive silicone composition and semiconductor device
WO2020241054A1 (en) 2019-05-27 2020-12-03 信越化学工業株式会社 Thermally-conductive silicone composition, semiconductor device, and production method therefor
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