鋇-硼-矽-鋁-氧化物玻璃系統於水基刮刀成形的製程、分析與應用之研究

本研究針對鋇-硼-矽-鋁-氧化物玻璃系統進行有關水基刮刀之製程、高溫黏度與潛變行為的分析、多層結構的燒結行為與界面反應進行探討。本研究的第一部分是藉由田口法來進行G1A5玻璃薄帶(莫耳比：46.55氧化鋇-27.86氧化矽-20.46氧化硼-5.12氧化鋁)水基刮刀成形之製程參數最佳化，並比較不同參數對翹曲量及燒結密度性質的相對重要性。另一方面，G6玻璃薄帶(莫耳比：31.99氧化鋇-44.49氧化矽-22.24氧化硼-1.27氧化鋁)之製程參數是以G1A5為基礎進行調整；兩者參數之間的差異與原因亦於本文中討論。本研究亦觀察G6玻璃薄帶於乾燥過程中因不恰當的製程參數所產生的缺陷與時間、厚度之關係。本研究的第二部分是將第一部分發展出的玻璃薄帶進行熱壓堆疊形成多層結構，探討當內部存在預留之氣體流道時，流道頂端因潛變所造成的塌陷量與溫度(T)、時間(t)及流道寬度(w)之關係；根據實驗的結果，提出一公式來預測塌陷量於其他T、t、w下的變化量。此外，利用壓印潛變技術來研究G1A5玻璃的高溫黏度、剪切應變與應力的關係、應力指數(n)與產生流變之活化能(Q)。實驗結果顯示G1A5玻璃在600-630oC表現出牛頓流體的行為，產生應變之活化能為444±1.5 kJ.mol-1。本研究的第三部分是探討各種不同G1A5/G6多層結構的燒結行為，以及針對銀電極與玻璃之間的界面反應進行研究。研究結果顯示，因G6玻璃相對G1A5具有較高之玻璃轉換溫度與軟化點之故，當G6與G1A5之間的界面數量增加時，G1A5的燒結收縮會受到界面的影響導致所需的時間延長。若將銀/玻璃複合材在550-750oC的導電度與純玻璃基板做比較可以發現，前者的導電度提升了7-8個數量級。於銀/玻璃介面處進行元素圖譜分析發現，在氧化條件下於750oC持溫4 hr之後仍沒有顯著的擴散反應。最後，本研究示範了利用噴墨技術將銀線噴在玻璃薄帶上的可行性；測試結果顯示銀墨水與G1A5或G6之潤濕性良好，銀線寬度最細可達56 um，但兩線之間距不宜小於66 um，否則會有局部重疊之現象。

關鍵字

水基；刮刀成形；玻璃；田口法；壓印潛變；燒結行為；界面分析

並列摘要

Processing, analysis and application of two BaO-B2O3-SiO2-Al2O3 glass tapes by water-based tape casting are researched in this study. In the first part, optimization of parameters for the processing of G1A5 (46.55BaO-27.86SiO2-20.46B2O3-5.12Al2O3, in mol %) glass tape is designed according to Taguchi method, which also helps realizing the relative significance of key variables. Eight different parameters (including type of dispersant, quantity of binder and plasticizer, content of solid loading, casting rate, sintering temperature and time for sintering) for warpage and sintered density are considered and optimized successfully. On the other hand, G6 (31.99BaO-44.49SiO2-22.24B2O3-1.27Al2O3, in mol %) glass tape is developed through modifying the formula used for G1A5 tape. Difference between the two formulas is discussed, and the formation of defects in G6 tape during drying is characterized with respect to time and thickness. In the second part, suitable condition of lamination using G1A5 glass tape as basic material is applied to stack various kinds of multi-layered glass structures. Quantitative slumping of interior channels with respect to time, temperature, and width of channel is analyzed, and a master equation is proposed to help predicting the amount of collapse when the above three parameters are available. On the other hand, investigation of rheological behavior of G1A5 glass used for IT-SOFC is conducted. Value of viscosity is measured indirectly by impression creep technique. Response of shear strain to corresponding shear stress is analyzed, which reveals that the glass system possesses Newtonian behavior at 600-630oC. Stress exponent and activation energy for viscous flow at different temperatures and stresses are also determined to be 1.0 and 444±1.5 kJ.mol-1, respectively. In the third part, sintering behaviors of various multi-layered G1A5/G6 glass substrate are investigated. In addition, the temperature-dependent electrical conductivities of G1A5/silver and G6/silver composites are measured and compared with pure glasses. Elemental mapping at the interface of G1A5/silver and G6/silver composites confirms that there is no apparent interaction between silver and glass after sintering and aging at 750oC for 4 hr. Glass tape with ink-jet printed Ag wire demonstrated as a preliminary study shows that the finest Ag wire can be achieved is about 56 um, while overlaps between two Ag wires tend to happen when they are printed with an interval smaller than 66 um.

並列關鍵字

aqueous ； tape casting ； glass ； Taguchi method ； impression creep ； sintering ； interfacial ； ink-jet printing

參考文獻

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鋇-硼-矽-鋁-氧化物玻璃系統於水基刮刀成形的製程、分析與應用之研究

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