KR880000654B1 - 금속-세라믹접합체 - Google Patents

금속-세라믹접합체 Download PDF

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KR880000654B1
KR880000654B1 KR1019850000734A KR850000734A KR880000654B1 KR 880000654 B1 KR880000654 B1 KR 880000654B1 KR 1019850000734 A KR1019850000734 A KR 1019850000734A KR 850000734 A KR850000734 A KR 850000734A KR 880000654 B1 KR880000654 B1 KR 880000654B1
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metal
ceramic
oxide layer
bonding
amorphous
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순이찌로오 다나까
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가부시끼 가이샤 도시바
사바 쇼오이찌
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Abstract

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Description

금속-세락믹 접합체
제1도 가열 온도에 따른 유리층 및 접합 강도의 변화를 나타낸 그래프.
제2도 유리상(相)과 접합강도의 관계를 나타낸 그래프.
본 발명은 금속 세라믹 접합체에 관한 것이다.
세라믹은 구조 재료로서 사용하는 시도가 요즈음 이루어 지고 있다.
이와 같은 경우에 세라믹을 다른 부재와 접합해서 사용하지 않으면 안되는 것이 많다.
이와 같은 세라믹과 다른 부재의 접합 수단으로서는 접착제에 의한 접합, 또는 세라믹을 몰리브덴-망간 등으로 금속화 한 뒤에 납땜하는 접합등이 이루어져 왔다.
그런데, 접착제로 인한 접합에서는 구조체로서 사용할 수 있는 온도 범위가 낮으며, 또한 금속화로 인한 접합은 금속화 할 수 있는 세라믹이 알루미나 등으로 한정되어서 질화 규소 등의 구조재로서 적합한 실리콘 세라믹에 그대로 적용할 수 없다는 문제점이 있었다.
본 발명은 상술한 접합강도가 큰 실리콘 세라믹과 금속의 접합체를 제공하는데 있다.
본 발명은 실리콘 세라믹을 주체로 하여 구성된 세라믹 부재와, 실리콘 세라믹 부재의 표면상에 결정 질상 및 비결정 질상으로된 산화물 층과, 상기 산화물층 내로 확산되어 산화물층과 접합되는 금속부재로 이루어진 것을 특징으로 한다.
실리콘 세라믹은 금속과의 접합에 도움이 되는 알루미늄을 Al2O3등의 형태로 함유하는 것이 좋고 또한 소결조제(燒結助劑)로서 Y2O3등의 희토류(希土類) 산화물을 함유한 것이 바람직하다.
또한 천이금속계(遷移金屬系) 산화물의 소결조제 및 알칼리 금속, 알칼리 토류금속, 천이금속계의 원소를 포함해도 좋다.
이것 들을 알루미늄과 조합시키므로서 금속과의 접합상태를 개선하는 효과가 있다고 생각된다.
또한, 실리콘 세라믹으로서는 Si3N4또는 Si-Al-O-N 과 같이 질소를 함유하는 것이 금속과의 결합상태를 양호하게 하는 점에서 바람직하다.
상술한 산화물층은 실리콘 세라믹을 산화시킨 것이며 비결정 질상으로서 알루미늄을 함유한 규산염 유리를 주성분으로 하여 구성된 것이 접합강도가 크다.
또한 결정 질상으로서는 α 홍연석(紅鉛石) 및 Y2O3·2SiO2를 함유하는 것이 좋다.
산화물층의 알루미늄량은 산화물충에 대하여 0.01-50 중량%의 범위에서 접합을 강화시키는 효과가 크다.
또한 산화물층은 0.2-30㎛의 두께로된 것이 바람직하다.
비결정 질상은 산화물층 가운데에서 20체적% 이상에서 부터 접합을 강화시키는 효과를 나타내며, 바람직하게는 50체적% 이상인 것이 좋다.
실리콘 세라믹과 금속과의 접합상태로서 금속은 주로 비결정 질상과 접합된 상태의 것이 바람직하고, 또한 접합형태는 띠 모양(帶狀) 또는 점 모양(點狀)의 것이 금속과 세라믹의 열팽창 차이로 인한 응력을 완화하는 점에서 바람직하다.
금속과 비결정 질상의 접합은 금속 및 금속산화물과 비결정 질상 사이의 고용, 화합물 생성 및 확산으로 이루어 진다.
이 경우에 금속과 금속산화물은 공정물(共晶物)인 것이 바람직하다.
이와 같은 접합상태를 얻으려면 금속으로서는 동 또는 동합금, 그 가운데에서도 터프피치 구리(tough pitch copper)가 바람직하다.
본 발명의 접합체를 얻으려면 우선, 실리콘 세라믹을 대기중에서 1200-1400℃로 20분-20시간 가열해서 실리콘 세라믹의 표면에 접합할 수 있는 층을 형성한다.
이 경우 표면에 생성되는 층은 주로 α 홍연석, Y2O3·2SiO2및 알루미늄을 함유한 규산염 유리로 구성된다.
이 가운데에서 접합하는데 크게 도움이 된다고 생각되는 것은 알루미늄을 함유한 규산염 유리이지만 Y2O3·2SiO2가 인편(鱗片) 형상의 결정이며 또한 결정의(110) 면을 표면에 대해서도 거의 평행으로 배향석출(配向析出)된 상태로 혼합되어 있는 것도 효과가 있다.
이렇게 해서 얻어진 실리콘 세라믹의 표면층에 금속을 맞닿게 하여 가열 처리한다.
예를 들어 터프 피치 구리라고 하면 불활성 분위기 속에서 1065-1083℃ 의 범위로 1분-2시간 가열처리 한다.
이 경우에 금속으로서는 미량의 산소(酸素) (80-3900 ppm)를 함유한 것이 좋지만, 그렇지 않은 경우는 가열 분위기에서 미량의 산소(수 100 ppm) 를 함유시키는 것이 유효하다.
Y2O35% (중량 %), Al2O34%, AlN 3%, TiO21.5% 를 함유한 Si3N4의 상압소결체(常
Figure kpo00001
燒結體)를 대기 중에서 1200-1400℃ 로 약 10시간 가열하여 표면에 금속과 결합할 수 있는 층을 형성하였다. (두께 5㎛).
얻어진 Si3N4표면을 X선 회절(回折)로 분석한 결과, Si3N4외에 Y2O3·2SiO2, α 홍연석 및 알루미늄을 함유한 유리상(규산염유리)이 발견되었다.
유리상은 산화물층 가운데 약 60체적% 이며 또한 산화물층 속의 알류미늄의 량은 약 20중량% 였다.
제1도는 가열온도에 따른 유리상량(相量)의 변화를 나타낸다. (곡선 A).
또한 그래프 중의 유리량은 임의 단위로 나타내지만, 이량은 금속과 세라믹의 접합층의 체적에서 차지하는 유리상량에 비레한 량이다.
이렇게 해서 얻어진 Si3N4에 터프피치구리판체를 맞닿게 하여 불활성 분위기 속에서 1075℃ 로 가열하는 직접 접합법으로 동판체를 접합하였다.
이 경우에 접합은 1065℃-1083℃ 의 온도로 행한다.
이 결과를 제1도에 합쳐서 나타낸다. (곡선 B).
이상으로 명백한 바와 같이 접합층에 유리상이 존재함으로서 접합강도는 향상된다.
또한, 가열 온도가 너무 높아지면 결정이 크고 거칠어져 강도면에서 바람직하지 않다.
세라믹의 가열처리 온도는 1250℃-1350℃ 의 범위에서 보다 바람직한 접합 강도를 얻을 수 있다.
유리량과 접합 강도의 관계를 제2도에 나타낸다.
제2도에서 유리량이 접합 강도에 도움이 되고 있는 것을 알 수 있다.
접합강도가 높은 것에 대하여 접합면의 관찰을 하였다.
접합면에 있어서 동은 주로 유리상과 접합해 있고, 또한 띠 모양이나 점 모양의 국부적 접합을 나타내고 있었다.
더우기, 접합부에 있어서 금속쪽은 동 산화물과 동의 공정물(共晶物)로 구성되어져 있고, 이것들과 세라믹쪽의 유리상과의 사이에서 고용(固溶)되거나 화합물을 생성하거나 또는 확산되므로서 견고한 접합이 되어있는 것이 확인 되었다.
이상과 같이 본 발명의 금속-세라믹 접합체는 신뢰할 수 있는 접합상태를 가지고 있는 것이다.
이어서, 본 발명의 바람직한 실시 형태를 나타내면 다음과 같다.
(1) 실리콘 세라믹은 Al2O3등의 형태로 알루미늄을 함유하는 것이어야 할것.
세라믹속에 함유되어 있는 알루미늄은 결합강도 개선에 도움이 된다.
(2) 실리콘 세라믹을 산화시킨 층속의 알루미늄량은 0.01-50 중량% 이어야 할것.
(3) 실리콘 세라믹은 Si3N4또는 Si-Al-O-N 등과 같이 질소를 함유하는 것이어야 할것.
이것들은 강도가 크며, 접합강도가 큰 것을 얻을 수 있다.
(4) Si3N4또는 Si-Al-O-N 등에 소결조제로서 Y2O3등의 회토류 산화물을 10중량% 이하로 함유할것.
소결체가 치밀화 되어져 강도 향상을 가져온다.
(5) 산화물층은 결정 질상으로서, α 홍연석, Y2O3·2SiO2를 함유하고 비결정 질상으로서 알루미늄을 함유한 규산염 유리를 함유한 것이어야 할것.
(6) 금속은 주로 비결정 질상과 접합해 있어야 할것.
(7) 금속과 비결정 질상의 접합상태는 띠 모양 또는 점 모양의 국부적 접합이어야 할것.
(8) 금속과 비결정 질상의 접합은 금속 또는 금속 산화물과 비결정 질상 사이의 고용(固溶), 화합물 생성 및 확산으로 인한 것이며, 금소과 금속 산화물은 공정물 이어야 할것.
(9) 금속은 동 또는 동합금이어야 할것.

Claims (7)

  1. 실리콘 세라믹을 주체로 하여 구성된 세라믹 부재와, 실리콘 세라믹 부재의 표면상에 결정 질상 및 비결정 질상으로된 산화물층과, 상기 산화물층 내로 확산되어 산화물층과 접합되는 금속부재로 이루어진 것을 특징으로 하는 금속-세라믹 접합체.
  2. 제1항에 있어서, 금속부재는 주로 비결정 질상과 접합하여된 것을 특징으로 하는 금속-세라믹 접합체.
  3. 제1항에 있어서, 금속과 비결정 질상의 접합은 금속 또는 금속 산화물과 비결정 질상 사이의 고용, 화합물 생성 및 확산에 따른 것임을 특징으로 하는 금속-세라믹 접합체.
  4. 제1항에 있어서, 실리콘 세라믹은 Si3N4또는 Si-Al-O-N 로 구성된 그룹으로 부터 선택되는 것을 특징으로 하는 금속-세라믹 접합체.
  5. 제4항에 있어서, 실리콘 세라믹은 소결조제로서 Y2O3을 10 wt% 이하로 함유하는 것을 특징으로 하는 금속-세라믹 접합체.
  6. 제4항에 있어서, 실리콘 세라믹은 주로 α-홍연석, Y2O3·2SiO2및, 알루미늄을 함유한 규산염 유리를 함유한 것을 특징으로 하는 금속-세라믹 접합체.
  7. 제2항에 있어서, 금속부재와 비결정 질상 사이의 접합상태는 띠 모양 또는 점 모양인 것을 특징으로 하는 금속-세라믹 접합체.
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