研究生: |
張瑞娟 Chang,Jui-Chuan |
---|---|
論文名稱: |
低溫自我束縛共燒陶瓷系統 Self-Constrained Sintering of Low Temperature Cofired Ceramic Systems |
指導教授: |
簡朝和
Jean,Jau-Ho |
口試委員: | |
學位類別: |
博士 Doctor |
系所名稱: |
工學院 - 材料科學工程學系 Materials Science and Engineering |
論文出版年: | 2008 |
畢業學年度: | 97 |
語文別: | 中文 |
論文頁數: | 220 |
中文關鍵詞: | 束縛燒結 、低溫共燒陶瓷 |
相關次數: | 點閱:3 下載:0 |
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本篇論文旨在探討自我束縛低溫共燒陶瓷的設計概念及材料於束縛燒結時的緻密行為。首先,於第一章先回顧低溫共燒陶瓷基板的發展歷程,及束縛燒結技術所遇到的問題。在第二章中,首先探討自我束縛燒結系統之構成材料La2O3-B2O3-CaO玻璃 Al2O3(LBCGA)的結晶動力學及其機制。此介電玻璃陶瓷系統在熱處理的過程中,會先後生成LaBO3與LaAl2.03(B4O10)O0.54結晶相。其中低溫結晶相LaBO3的生成時機對系統的緻密行為影響甚鉅,而由Avrami分析法所得之Avrami指數與結晶活化能的分析結果可判定LaBO3結晶為三維的介面反應所控制,而此結論由非等溫的DTA分析法與晶體成長速率的結果得到進一步的確認。
接著,在第三章中,藉由理論的推導與適當的實驗設計成功地將LBCGA於自由及束縛燒結時的單軸向黏度值精確地量測出來,且準確地計算出使LBCGA於束縛燒結時的緻密速率與自由燒結時相同,所需施加的外加應力值。LBCGA於自由及束縛燒結時的單軸向黏度值在LaBO3結晶產生前皆隨著溫度的升高而呈現下降的趨勢,唯束縛燒結時的黏度值較自由燒結時來得大。由燒結活化能及平面張應力的分析結果顯示,LBCGA的緻密機制並沒有因為外加的張應力而發生改變,仍為黏滯流動所控制,而造成LBCGA於束縛燒結時緻密速率下降的原因乃束縛燒結所產生的平面張應力阻礙了材料的流動,使得整體的黏度提高,緻密速率因而變慢。
在第四章中,由LBCGA生胚薄片及Al2O3生胚薄片所組成之自我束縛低溫共燒陶瓷系統被成功地研發出來。由於Al2O3的燒結溫度遠高於LBCGA,因此當LBCGA燒結時,尚未燒結之Al2O3層可有效地阻止LBCGA層於側向上的收縮,而待溫度繼續升高,LBCGA層中經結晶後所殘餘之玻璃相開始藉由毛細作用力滲透進入Al2O3層中使之緻密化,此時已緻密且結晶之LBCGA可有效地阻止Al2O3層於側向上的收縮,如此交互束縛的結果使得LBCGA/Al2O3自我束縛系統在整個共燒的過程中僅於x、y方向產生約0.6%的微量收縮。由活化能的量測結果顯示玻璃滲透進入Al2O3層的行為乃受玻璃的黏滯流動所控制,而利用理論計算各溫度下不同厚度之Al2O3生胚滲透所需的時間與實驗量測值相近。然而,當玻璃的滲透層太厚時,則會導致LBCGA層出現去緻密化的現象。
在第五章中,探討構成自我束縛燒結系統的另一組成材料 BaO-CaO-TiO2-SiO2玻璃 Zn2SiO4 Al2O3(BZA)於束縛燒結時的緻密行為。BZA於束縛與自由燒結時之單軸向黏度值隨溫度變化的趨勢和LBCGA相同,皆隨著燒結溫度的提高而呈現下降的趨勢,且束縛燒結時的黏度值亦較自由燒結時來得大。經由燒結活化能及平面張應力的量測,顯示束縛燒結時黏度值上升的主因亦來自於束縛燒結所產生的平面張應力阻礙了材料的流動所致。雖然BZA於束縛燒結時的緻密速率因平面張應力的影響而較自由燒結時來得緩慢,但是在玻璃結晶溫度與玻璃轉化溫度間的溫度範圍足夠大的條件下,使得BZA系統無論於自由燒結抑或是束縛燒結時皆能達到極佳的緻密度。反觀LBCGA於束縛燒結時則需升溫速率高於10℃/min的情形下才可達到緻密。
最後,為了改善LBCGA/Al2O3自我束縛燒結系統因玻璃滲透而導致LBCGA產生去緻密化的情形,因此改以BZA取代Al2O3的方式另行設計出LBCGA/BZA自我束縛燒結系統。由於LBCGA和BZA的燒結溫度區間沒有重疊,因此在共燒的過程中彼此可以交互扮演束縛層的角色,使LBCGA/BZA多層結構在共燒後僅在x軸向產生約1%的微量收縮。此外,因LBCGA及BZA乃利用系統本身含有的玻璃來達到緻密化,並不需依賴另一方的供給,因此可有效地避免如LBCGA/Al2O3自我束縛燒結系統因玻璃滲透而導致LBCGA產生去緻密化的問題。此外,由於LBCGA/BZA共燒時所產生的不匹配應力遠小於燒結驅動力,因此試片在共燒後並沒有觀察到有脫層和破裂等缺陷產生。
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