JPH0627035B2 - Method for manufacturing aluminum nitride sintered body - Google Patents
Method for manufacturing aluminum nitride sintered bodyInfo
- Publication number
- JPH0627035B2 JPH0627035B2 JP63121928A JP12192888A JPH0627035B2 JP H0627035 B2 JPH0627035 B2 JP H0627035B2 JP 63121928 A JP63121928 A JP 63121928A JP 12192888 A JP12192888 A JP 12192888A JP H0627035 B2 JPH0627035 B2 JP H0627035B2
- Authority
- JP
- Japan
- Prior art keywords
- aluminum nitride
- firing
- thermal conductivity
- sintered body
- furnace
- 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 - Lifetime
Links
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 title claims description 30
- 238000004519 manufacturing process Methods 0.000 title claims description 6
- 238000000034 method Methods 0.000 title description 6
- 238000010304 firing Methods 0.000 claims description 34
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 26
- 229910052799 carbon Inorganic materials 0.000 claims description 23
- 238000005245 sintering Methods 0.000 claims description 16
- 239000012298 atmosphere Substances 0.000 claims description 15
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims description 14
- 229910052721 tungsten Inorganic materials 0.000 claims description 14
- 239000010937 tungsten Substances 0.000 claims description 14
- 239000000463 material Substances 0.000 claims description 7
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 4
- 229910052750 molybdenum Inorganic materials 0.000 claims description 4
- 239000011733 molybdenum Substances 0.000 claims description 4
- 230000001590 oxidative effect Effects 0.000 claims description 3
- 239000000843 powder Substances 0.000 description 17
- 238000010438 heat treatment Methods 0.000 description 15
- 230000000052 comparative effect Effects 0.000 description 10
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 8
- 239000001301 oxygen Substances 0.000 description 8
- 229910052760 oxygen Inorganic materials 0.000 description 8
- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 description 7
- 239000012071 phase Substances 0.000 description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- 229910018072 Al 2 O 3 Inorganic materials 0.000 description 5
- 150000001875 compounds Chemical class 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- BRPQOXSCLDDYGP-UHFFFAOYSA-N calcium oxide Chemical compound [O-2].[Ca+2] BRPQOXSCLDDYGP-UHFFFAOYSA-N 0.000 description 3
- ODINCKMPIJJUCX-UHFFFAOYSA-N calcium oxide Inorganic materials [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 3
- 239000000292 calcium oxide Substances 0.000 description 3
- 239000000470 constituent Substances 0.000 description 3
- 229910002804 graphite Inorganic materials 0.000 description 3
- 239000010439 graphite Substances 0.000 description 3
- 238000000465 moulding Methods 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- 230000009467 reduction Effects 0.000 description 3
- 229940105963 yttrium fluoride Drugs 0.000 description 3
- RBORBHYCVONNJH-UHFFFAOYSA-K yttrium(iii) fluoride Chemical compound F[Y](F)F RBORBHYCVONNJH-UHFFFAOYSA-K 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 2
- JNDMLEXHDPKVFC-UHFFFAOYSA-N aluminum;oxygen(2-);yttrium(3+) Chemical compound [O-2].[O-2].[O-2].[Al+3].[Y+3] JNDMLEXHDPKVFC-UHFFFAOYSA-N 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000001257 hydrogen Substances 0.000 description 2
- 229910052739 hydrogen Inorganic materials 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- -1 rare earth compounds Chemical class 0.000 description 2
- 229910052761 rare earth metal Inorganic materials 0.000 description 2
- 229910018516 Al—O Inorganic materials 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000002411 adverse Effects 0.000 description 1
- 229910052784 alkaline earth metal Inorganic materials 0.000 description 1
- 150000001341 alkaline earth metal compounds Chemical class 0.000 description 1
- 150000001342 alkaline earth metals Chemical class 0.000 description 1
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 239000012752 auxiliary agent Substances 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 238000000280 densification Methods 0.000 description 1
- 239000012535 impurity Substances 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 150000001247 metal acetylides Chemical class 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 238000005121 nitriding Methods 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000006104 solid solution Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/515—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics
- C04B35/58—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides
- C04B35/581—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on borides, nitrides, i.e. nitrides, oxynitrides, carbonitrides or oxycarbonitrides or silicides based on aluminium nitride
Landscapes
- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Ceramic Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
- Structural Engineering (AREA)
- Organic Chemistry (AREA)
- Ceramic Products (AREA)
Description
【発明の詳細な説明】 〔産業上の利用分野〕 本発明は、高い熱伝導性を有する窒化アルミニウム焼結
体の製造方法に関する。The present invention relates to a method for manufacturing an aluminum nitride sintered body having high thermal conductivity.
〔従来の技術〕 窒化アルミニウムは、理論熱伝導率が３２０ｗ／m・kと
高くはあるが、従来、原料となる窒化アルミニウム粉の
純度が低かつたこと、さらには効果的な焼結助剤が見い
出せなかつたこと等により、その熱伝導率は１００ｗ／
m・kを下廻つていた。近年、直接窒化法、アルミナ還元
法等の窒化アルミニウム粉の製造方法を問わず、その高
純度化には著しいものがあり、さらに焼結助剤として、
希土類化合物、アルカリ土類金属化合物等、本来の焼結
助剤の役割の他に、不純物酸素の捕獲剤として働く添加
剤も見い出されるに至り、焼結体の熱伝導率も２００ｗ
／m・k近くまで達している。しかしながら、窒化アルミ
ニウムのもつ理論熱伝導率を考えると、従来の方法より
得られている焼結体の熱伝導率は未だ半分をわずかに超
えるに過ぎず、より熱伝導性の優れた焼結体の開発が望
まれている。[Prior Art] Aluminum nitride has a high theoretical thermal conductivity of 320 w / m · k, but conventionally, the purity of the raw material aluminum nitride powder was low, and further, an effective sintering aid. The thermal conductivity is 100w /
It was below m ・ k. In recent years, regardless of the production method of aluminum nitride powder such as direct nitriding method and alumina reduction method, there is a remarkable increase in its purification, and further as a sintering aid,
In addition to the original role of sintering aids such as rare earth compounds and alkaline earth metal compounds, additives that act as scavengers for impurity oxygen have also been found, and the thermal conductivity of sintered bodies is 200 w.
/ Nearly m ・ k is reached. However, considering the theoretical thermal conductivity of aluminum nitride, the thermal conductivity of the sintered body obtained by the conventional method is still only slightly over half, and the sintered body with higher thermal conductivity is obtained. Development is desired.
本発明者らは、上記の問題点を解決するため鋭意検討を
重ねた結果、窒化アルミニウムを主成分とする成形体を
焼成するに際し、焼成雰囲気が、その焼結体の熱伝導率
を大きく左右することを見い出し、本発明を完成した。As a result of intensive studies to solve the above problems, the present inventors have found that when firing a molded body containing aluminum nitride as a main component, the firing atmosphere greatly affects the thermal conductivity of the sintered body. As a result, they have completed the present invention.
即ち、本発明は、窒化アルミニウムと焼結助剤を含む成
形体を焼成するに際し、炭素雰囲気又は炭素を含む雰囲
気を発生しない焼成炉を用い、非酸化性雰囲気中で焼成
すること、特に焼成炉として、発熱体がタングステンで
あり、炉材がタングステン又はタングステンとモリブデ
ンからなるものを使用することを特徴とする窒化アルミ
ニウム焼結体の製造方法である。That is, the present invention uses a firing furnace that does not generate a carbon atmosphere or an atmosphere containing carbon when firing a molded body containing aluminum nitride and a sintering aid, and particularly performs firing in a non-oxidizing atmosphere. In the method for producing an aluminum nitride sintered body, the heating element is tungsten, and the furnace material is tungsten or tungsten and molybdenum.
以下、本発明をさらに詳細に説明する。Hereinafter, the present invention will be described in more detail.
本発明者らは、窒化アルミニウム粉に焼結助剤を添加後
成形し焼成した窒化アルミニウム焼結体の構成相と熱伝
導率の関係を詳細に検討したところ、添加した焼結助剤
が窒化物や炭化物になると、熱伝導率が最早向上しなく
なることを見い出すとともに、それら窒化物や炭化物が
生成される主要な原因は成形体を焼成する焼成炉、すな
わち発熱体並びに炉材が炭素質のものを使用しているた
めであることを見い出したものである。すなわち、窒化
アルミニウムは、難焼結生物質であるため、焼結助剤を
添加したとしても、その焼成温度が高いため、従来から
黒鉛を発熱体とした炉が用いられてきたが、高温におい
て、発熱体並びに炉材から飛散する炭素雰囲気又は炭素
有雰囲気のため、成形体に悪影響を及ぼし、熱伝導率の
向上が頭打ちとなることを見い出したのである。The present inventors have studied in detail the relationship between the constituent phase and the thermal conductivity of an aluminum nitride sintered body obtained by adding a sintering aid to aluminum nitride powder, followed by molding and firing. In addition to finding that the thermal conductivity no longer improves when it becomes a substance or a carbide, the main cause of the formation of these nitrides and carbides is the firing furnace for firing the molded body, that is, the heating element and the furnace material I found that it was because I was using something. That is, since aluminum nitride is a difficult-to-sinter raw material, even if a sintering aid is added, its firing temperature is high, so that a furnace using graphite as a heating element has been conventionally used. It has been found that the carbon atmosphere or the carbon-containing atmosphere scattered from the heating element and the furnace material adversely affects the molded body, and the improvement of the thermal conductivity reaches the ceiling.
ここで、酸化イットリウムを添加した成形体を例にあげ
て詳しく説明すると、酸化イットリウムは窒化アルミニ
ウムの熱伝導率を向上させる代表的な焼結助剤であり、
この助剤は、窒化アルミニウム粉表面上に不可避的に存
在する酸素と反応し、イットリウムアルミネートの液相
を生成させ、成形体の緻密化を促がすとともに、3Y2O3・
5Al2O3、Y2O3・Al2O3、2Y2O3・Al2O3等の化合物を形成せ
しめることにより酸素の窒化アルミニウム粒子内への固
溶を抑えて、高い熱伝導性を有する焼結体を形づくるも
のである。Here, a detailed description will be given by taking a molded body to which yttrium oxide is added as an example. Yttrium oxide is a typical sintering aid for improving the thermal conductivity of aluminum nitride,
This auxiliary agent reacts with oxygen unavoidably present on the surface of the aluminum nitride powder to generate a liquid phase of yttrium aluminate, promotes densification of the molded body, and 3Y 2 O 3
By forming compounds such as 5Al 2 O 3 , Y 2 O 3 · Al 2 O 3 and 2Y 2 O 3 · Al 2 O 3 , the solid solution of oxygen in aluminum nitride particles is suppressed and high thermal conductivity is achieved. To form a sintered body having.
本発明者らは、窒化アルミニウムと酸化イットリウムか
らなる成形体を焼成するに際し、2Y2O3・Al2O3を生成さ
せ、さらに焼成時間等を伸ばし前記化合物の変化と熱伝
導率の関係を検討したところ、前記化合物が2Y2O3・Al2O
3からY2O3と2Y2O3・Al2O3、さらにＹＮとY2O3へとイット
リウムアルミネート相が還元されていること、この還元
に伴ない熱伝導率が少しずつ向上すること、及びＹＮが
生成した時点から熱伝導率が低下し始めること等を確認
するとともに、これらの還元を起こさせている原因は黒
鉛質の発熱体並びに炉材から飛散する炭素又は炭素を含
む雰囲気であることを見い出したものである。The present inventors, when firing a molded body made of aluminum nitride and yttrium oxide, to generate 2Y 2 O 3 · Al 2 O 3 , further extend the firing time, etc. to show the relationship between the change of the compound and the thermal conductivity. Upon examination, it was found that the compound was 2Y 2 O 3 .Al 2 O.
The yttrium aluminate phase is reduced from 3 to Y 2 O 3 and 2Y 2 O 3 · Al 2 O 3 , and further to YN and Y 2 O 3 , and the thermal conductivity gradually improves with this reduction. And the fact that the thermal conductivity begins to drop from the time when YN is generated, and the cause of causing these reductions is the graphite heating element and the carbon or carbon-containing atmosphere scattered from the furnace material. It was found that.
ＹＮが生成するとなぜ熱伝導率が向上しなくなるかにつ
いては未だ明らかではないが、上記還元ガスを発生しな
い焼結炉、例えばタングステンを発熱体並びに炉材とし
たものを使用すると、従来の黒鉛質炉では１７０ｗ／m・
kであつたものが同じ焼成温度時間で２００ｗ／m・k、ま
た従来200ｗ／m・kのものが２３５ｗ／m・kを超える熱伝
導率にすることができる。Although it is not clear yet why the thermal conductivity does not improve when YN is generated, when a sintering furnace that does not generate the above-mentioned reducing gas, for example, a heating element and a furnace material of tungsten is used, 170 w / m in the furnace
It is possible to obtain a thermal conductivity of 200 w / m · k in the same firing temperature time of 200 k / k, and 235 w / m · k in the conventional 200 w / m · k.
このように熱伝導率が向上する原因は、酸化イツトリウ
ムの場合、結果的にはＹＮが生成しないこと、すなわ
ち、従来の黒鉛炉においては、熱伝導率を向上させる
相、例えば2Y2O3・Al2O3を形成させたのち、さらにその
効果を高めるために加熱処理の時間を伸ばしてもかえつ
てＹＮの生成を促がし、本来のY-Al-O相の効果を発現さ
せられなかつたのに対し、本発明のように、炭素又は炭
素含有ガスを発生しない炉の使用により、その効果を充
分に発揮できたためと考えている。In the case of yttrium oxide, the reason why the thermal conductivity is improved is that YN is not produced as a result, that is, in the conventional graphite furnace, a phase that improves the thermal conductivity, such as 2Y 2 O 3 ·. After forming Al 2 O 3 and extending the heat treatment time to further enhance the effect, the formation of YN is promoted and the original effect of the Y-Al-O phase cannot be expressed. On the other hand, it is considered that the use of a furnace that does not generate carbon or a carbon-containing gas, as in the present invention, was able to sufficiently exert its effect.
本発明は、上記のように、焼成助剤として酸化イツトリ
ウムの場合を例にして説明したが、これらのことは他の
焼結助剤例えば希土類元素を含む化合物やアルカリ土類
金属を含む化合物を添加した場合についても同様であ
る。Although the present invention has been described with reference to the case of yttrium oxide as the firing aid as described above, these may be applied to other sintering aids such as a compound containing a rare earth element or a compound containing an alkaline earth metal. The same applies when added.
本発明で使用する焼成炉としては、炭素雰囲気又は炭素
を含む雰囲気を発生しない炉であればいずれでもよい
が、窒化アルミニウム成形体の焼成雰囲気並びにその温
度を考慮した場合、発熱体がタングステンであり、炉材
としてタングステン又はタングステンとモリブテンとか
らなる構造のものが好適である。また、本発明におい
て、非酸化性雰囲気中とは、窒素、アルゴン、水素及び
これらの混合ガスをさすものである。これらのうち、特
に、窒素又は窒素と水素の混合ガスを使用することが好
ましい。焼成温度は、原料窒化アルミニウム粉の粒度や
添加する焼結助剤により異なつているが、１６００〜２
１００℃にて焼成することが好ましい。１６００℃より
低温にて焼成すると、成形体の緻密化が困難となり、一
方、２１００℃を超える温度での焼成は窒化アルミニウ
ムの分解が顕著になつて望ましくない。The firing furnace used in the present invention may be any furnace as long as it does not generate a carbon atmosphere or an atmosphere containing carbon, but in consideration of the firing atmosphere of the aluminum nitride molded body and the temperature thereof, the heating element is tungsten. It is preferable that the furnace material has a structure of tungsten or tungsten and molybdenum. Further, in the present invention, the term “in a non-oxidizing atmosphere” refers to nitrogen, argon, hydrogen and a mixed gas thereof. Of these, it is particularly preferable to use nitrogen or a mixed gas of nitrogen and hydrogen. The firing temperature varies depending on the particle size of the raw material aluminum nitride powder and the sintering aid to be added.
Baking at 100 ° C. is preferable. Firing at a temperature lower than 1600 ° C makes it difficult to densify the molded body, while firing at a temperature higher than 2100 ° C is not desirable because decomposition of aluminum nitride becomes remarkable.
以下、本発明を実施例と比較例をあげてさらに具体的に
説明する。Hereinafter, the present invention will be described more specifically with reference to Examples and Comparative Examples.
実施例１〜４、比較例１〜４ 酸素含有量が１．０重量％である窒化アルミニウム粉１
００重量部に酸化イツトリウムを４ないし６重量部添加
した粉末を充分混合した後、圧力３００kg／cm2の一軸
加圧成形をした。この成形体をさらに圧力１０００kg／
cm2のもとでラバープレスし、３０mmφ×５mmｔの円板
状成形体を得た。この成形体を、タングステンを発熱体
とし、その周囲にリフレクターとしてタングステンを用
いた焼成炉で、各々、N2中で１９００℃、１hr及び４hr
常圧焼結した。得られた焼結体を１０mmφ×３mmｔに研
削後、粉末Ｘ線回析法にてその相を同定するとともに、
密度を測定後、レーザーフラツシュ法にて熱伝導率を測
定した。Examples 1 to 4, Comparative Examples 1 to 4 Aluminum nitride powder 1 having an oxygen content of 1.0% by weight.
After thoroughly mixing the powder obtained by adding 4 to 6 parts by weight of yttrium oxide to 00 parts by weight, uniaxial pressure molding with a pressure of 300 kg / cm 2 was performed. This molded body is further pressure 1000kg /
Rubber pressing was performed under cm 2 to obtain a disk-shaped molded body of 30 mmφ × 5 mmt. This compact was placed in a firing furnace in which tungsten was used as a heating element and tungsten was used as a reflector around it in N 2 at 1900 ° C. for 1 hr and 4 hr, respectively.
Sintered under normal pressure. The obtained sintered body was ground to 10 mmφ × 3 mmt, and its phase was identified by powder X-ray diffraction method.
After measuring the density, the thermal conductivity was measured by the laser flash method.
比較のため、同一の成形体をカーボンを発熱体とした焼
成炉で窒化アルミニウムに包埋したこと以外は同一条件
で常圧焼結した。For comparison, the same compact was sintered under normal pressure under the same conditions except that it was embedded in aluminum nitride in a firing furnace using carbon as a heating element.
それらの結果を表１に示す。The results are shown in Table 1.
実施例５〜８、比較例５〜８ 酸素含有量が１．２重量％である窒化アルミニウム粉１
００重量部に酸化イツトリウムを５ないし７重量部添加
した粉末につき、実施例１と同様な方法にて成形体を作
製した。 Examples 5-8, Comparative Examples 5-8 Aluminum nitride powder 1 having an oxygen content of 1.2% by weight.
With respect to the powder obtained by adding 5 to 7 parts by weight of yttrium oxide to 00 parts by weight, a molded body was produced in the same manner as in Example 1.
この成形体を、発熱体としてタングステン、リフレクタ
ーとしてタングステンとモリブデンから成る焼成炉に
て、N2中、１８００℃にし３hr及び６hr常圧焼結を行な
つた。比較例として、同一の成形体をカーボンを発熱体
とした焼成炉を用い、表面をＢＮ粉でおおつたカーボン
ルツボ中に充填したこと以外は同一条件で常圧焼結し
た。The compact was subjected to normal pressure sintering for 3 hours and 6 hours in N 2 at 1800 ° C. in a firing furnace composed of tungsten as a heating element and tungsten and molybdenum as a reflector. As a comparative example, sintering was carried out under normal pressure under the same conditions except that a firing furnace in which the same compact was used as a heating element of carbon was used and the surface was filled in a carbon crucible covered with BN powder.
得られた焼結体の構成相、密度ならびに熱伝導率の測定
結果を表２に示す。Table 2 shows the measurement results of the constituent phase, density and thermal conductivity of the obtained sintered body.
実施例９〜１２、比較例９〜１２ 酸素含有量が０．９重量％である窒化アルミニウム粉１
００重量部にフツ化イツトリウムを５ないし７重量部添
加した粉末について実施例１と同様な方法により成形体
を作製した。この成形体を実施例１に示したものと同じ
焼成炉を用い、N2中１９００℃で２hrないし６hr常圧焼
結した。比較例として、同一の成形体をカーボンを発熱
体とした焼成炉を用い、カーボンルツボ中、ＢＮ粉末に
包埋したこと以外は同一条件で常圧焼結した。 Examples 9-12, Comparative Examples 9-12 Aluminum nitride powder 1 having an oxygen content of 0.9% by weight.
A powder was prepared by adding 5 to 7 parts by weight of yttrium fluoride to 00 parts by weight in the same manner as in Example 1 to prepare a molded body. This compact was sintered in N 2 at 1900 ° C. for 2 hr to 6 hr at atmospheric pressure using the same firing furnace as used in Example 1. As a comparative example, a firing furnace in which the same compact was used as a heating element of carbon was used and sintered under normal pressure under the same conditions except that it was embedded in BN powder in a carbon crucible.
得られた焼結体の構成相、密度及び熱伝導率の測定結果
を表３に示す。Table 3 shows the measurement results of the constituent phases, the density and the thermal conductivity of the obtained sintered body.
実施例１３〜１４、比較例１３〜１４ 酸素含有量が１．５重量％である窒化アルミニウム粉１
００重量部、フツ化イツトリウム３重量部さらに酸化カ
ルシウム１重量部からなる成形体（実施例１３）ならび
にフツ化イツトリウム２重量部、酸化カルシウム１．５
重量部からなる成形体（実施例１４）各々を実施例２と
同じ焼成炉中、N2雰囲気下、１９５０℃にて５hr焼成
し、焼結体を作製した。比較例として、同一の成形体を
カーボンを発熱体とした焼成炉を用い、カーボンルツボ
中、ＢＮ粉末に包埋したこと以外は同一条件で常圧焼結
した。 Examples 13-14, Comparative Examples 13-14 Aluminum nitride powder 1 having an oxygen content of 1.5% by weight.
00 parts by weight, yttrium fluoride 3 parts by weight and calcium oxide 1 part by weight (Example 13), and yttrium fluoride 2 parts by weight, calcium oxide 1.5.
Each of the compacts (Example 14) composed of parts by weight was fired in the same firing furnace as in Example 2 at 1950 ° C. for 5 hours in a N 2 atmosphere to produce a sintered body. As a comparative example, a firing furnace in which the same compact was used as a heating element of carbon was used and sintered under normal pressure under the same conditions except that it was embedded in BN powder in a carbon crucible.
焼結体の密度と熱伝導率の測定結果を表４に示す。Table 4 shows the measurement results of the density and the thermal conductivity of the sintered body.
実施例１５〜１６、比較例１５〜１６ 酸素含有量が１．２重量％である窒化アルミニウム粉１
００重量部に酸化カルシウムを１．０ないし１．５重量
部添加し、実施例１と同様な方法にて成形後、実施例１
に示す焼成炉を用いN2中、１８５０℃、４hr常圧焼結し
た。比較例として、同一の成形体をカーボンを発熱体と
した焼成炉を用い、表面をＢＮ粉でおおつたカーボンル
ツボ中に充填したこと以外は同一条件条件で常圧焼結し
た。Examples 15 to 16 and Comparative Examples 15 to 16 Aluminum nitride powder 1 having an oxygen content of 1.2% by weight.
To 100 parts by weight of calcium oxide was added 1.0 to 1.5 parts by weight, and after molding in the same manner as in Example 1, Example 1
Sintering was carried out in N 2 at 1850 ° C. for 4 hours under normal pressure using the firing furnace shown in FIG. As a comparative example, sintering was carried out under normal conditions under the same conditions except that a firing furnace in which the same compact was used as a heating element of carbon was used and the surface was filled in a carbon crucible covered with BN powder.
得られた焼結体の密度と熱伝導率の測定結果を表４に示
す。Table 4 shows the measurement results of the density and the thermal conductivity of the obtained sintered body.
（発明の効果） 本発明のように、窒化アルミニウムと焼結助剤を含む成
形体を、炭素や炭素を含む雰囲気を発生しない焼成炉に
て焼成することにより、熱伝導性に優れた窒化アルミニ
ウム焼結体を製造することができる。 (Effects of the Invention) As in the present invention, aluminum nitride excellent in thermal conductivity is obtained by firing a molded body containing aluminum nitride and a sintering aid in a firing furnace that does not generate carbon or an atmosphere containing carbon. A sintered body can be manufactured.
Claims (2)
成形体を焼成するに際し、炭素雰囲気又は炭素を含む雰
囲気を発生しない焼成炉を用い、非酸化性雰囲気中で焼
成することを特徴とする窒化アルミニウム焼結体の製造
方法。1. When firing a molded body containing aluminum nitride and a sintering aid, the firing is performed in a non-oxidizing atmosphere using a firing furnace that does not generate a carbon atmosphere or an atmosphere containing carbon. Method for producing aluminum nitride sintered body.
り、炉材がタングステン又はタングステンとモリブデン
からなるものを使用することを特徴とする特許請求の範
囲第(1)項記載の窒化アルミニウム焼結体の製造方法。2. An aluminum nitride sintered body according to claim 1, wherein the firing furnace is made of tungsten and the furnace material is made of tungsten or tungsten and molybdenum. Body manufacturing method.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63121928A JPH0627035B2 (en) | 1988-05-20 | 1988-05-20 | Method for manufacturing aluminum nitride sintered body |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63121928A JPH0627035B2 (en) | 1988-05-20 | 1988-05-20 | Method for manufacturing aluminum nitride sintered body |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH01294579A JPH01294579A (en) | 1989-11-28 |
| JPH0627035B2 true JPH0627035B2 (en) | 1994-04-13 |
Family
ID=14823392
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63121928A Expired - Lifetime JPH0627035B2 (en) | 1988-05-20 | 1988-05-20 | Method for manufacturing aluminum nitride sintered body |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0627035B2 (en) |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4578234A (en) * | 1984-10-01 | 1986-03-25 | General Electric Company | Process of pressureless sintering to produce dense high thermal conductivity ceramic body of deoxidized aluminum nitride |
| JPS61252481A (en) * | 1985-05-02 | 1986-11-10 | 東芝セラミツクス株式会社 | Baking device for ceramics |
-
1988
- 1988-05-20 JP JP63121928A patent/JPH0627035B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH01294579A (en) | 1989-11-28 |
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