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研究生: 葉勁宏
Jing-Hong Yeh
論文名稱: 固態氧化物燃料電池封裝玻璃與金屬連接板接合件高溫耐久機械性質分析
Analysis of High-Temperature Mechanical Durability for the Joint of Glass Ceramic Sealant and Metallic Interconnect for Solid Oxide Fuel Cell
指導教授: 林志光
Chih-Kuang Lin
口試委員:
學位類別: 碩士
Master
系所名稱: 工學院 - 機械工程學系
Department of Mechanical Engineering
畢業學年度: 99
語文別: 英文
論文頁數: 92
中文關鍵詞: 固態氧化物燃料電池玻璃陶瓷金屬連接板
外文關鍵詞: Solid Oxide Fuel Cell, Glass Ceramic Sealant, Interconnect
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  • 本研究主旨在探討經過不同時效處理之封裝玻璃陶瓷燒結試片,在不同測試溫度下(25 oC-800 oC)的機械強度與破壞模式,並評估含La0.67Sr0.33MnO3(LSM)塗層之金屬連接板與封裝玻璃陶瓷接合件於800 oC下之高溫機械強度。此外,也探討玻璃陶瓷和未含LSM塗層金屬連接板接合件於800 oC下的潛變性質。
    實驗結果顯示,經過1000 小時時效處理後之玻璃陶瓷燒結試片,於650 oC-750 oC下之抗折強度比在25 oC高,此乃由於裂縫癒合效應所致,而於800 oC下的強度為最低。另外,無論測試溫度高低,經過1000 小時時效處理之玻璃陶瓷試片強度優於100 小時時效處理之試片,而未經時效處理之試片強度為三者最低,此乃時效時間越長,結晶化程度越高,玻璃陶瓷之強度也就越高。
    有關玻璃陶瓷與含有LSM 塗層之金屬連接板的高溫機械性質與破壞模式,結果顯示含有LSM 塗層的接合件試片,其張力強度和剪力強度皆遠低於未含LSM 塗層的接合件試片,此乃由於鉻酸鋇層產生微孔洞以及微裂縫所致。由微結構及破斷面分析結果發現含有LSM 塗層的接合試片破壞皆發生於玻璃陶瓷基材與鉻酸鋇層的界面。未含LSM 塗層之剪力試片破壞則發生於玻璃基材內部並伴隨鉻酸鋇層的剝落,而未含LSM 塗層之張力試片破壞則發生於玻璃陶瓷基材內部。
    潛變接合件試片於800 oC下的潛變壽命會隨著負載減少而增加。在剪力試片方面,在1000 小時壽命的潛變強度約為剪力接合件強度的五分之一,而張力試片在1000 小時壽命的潛變強度則約為張力接合件強度的百分之八。另外,剪力試片在較短潛變壽命的破壞模式會與接合件強度測試的破壞模式相似,破壞皆發生在玻璃基材與鉻酸鋇層的界面,而較長潛變壽命試件的破壞則發生於玻璃基材內部並伴隨鉻酸鋇層的剝落,張力潛變試片破壞皆發生在玻璃基材與鉻酸鋇層的界面。


    Mechanical properties at various temperatures (25 oC-800 oC) were investigated for a newly developed solid oxide fuel cell glass sealant (GC-9) in variously aged conditions. The joint strength between the GC-9 glass-ceramic sealant and an interconnect steel (Crofer 22 H) coated with La0.67Sr0.33MnO3 (LSM) was also investigated at 800 oC. In addition, creep rupture properties of the joint specimens were also investigated at 800 oC under constant loading. For the 1000 h-aged, sintered GC-9 glass, the flexural strength at 650 oC-750 oC was greater than that at 25 oC due to a crack healing effect. From the force-displacement curves of the 1000 h-aged GC-9 glass, the inferred glass transition temperature (Tg) was between 750 oC and 800 oC. Therefore, its flexural strength was significantly reduced at 800 oC due to a viscous effect. However, a greater flexural strength and stiffness of the
    aged GC-9 glass over the non-aged one was observed at temperature higher than 700 oC due to a greater extent of crystallization. Both the shear and tensile bonding strength at 800 oC of the joint specimens coated
    with LSM were weaker than those of the non-coated ones. Through analysis of the interfacial microstructure, microvoids and microcracks were found at the BaCrO4
    chromate layer. When the LSM coating film and BaCrO4 layer were joined together with incompatible deformation, microvoids/microcracks were formed at the BaCrO4
    The creep rupture time of both shear and tensile joint specimens was increased with a decrease in the applied constant load at 800 layer. In this regard, the joint strength was degraded by such a coating. oC. The creep strength at 1000 h under shear loading was about one fifth of the shear strength at 800 oC. The tensile creep strength at 1000 h was about 8% of the tensile strength at 800 oC. The failure pattern of the shear creep joint specimens with a shorter creep rupture time was similar to that of the shear joint strength test specimens while a different failure pattern was found for a longer creep
    rupture time.

    LIST OF TABLES............................................................................................................ VIII LIST OF FIGURES............................................................................................................. NOMENCLATURE IX ...........................................................................................................XII 1. INTRODUCTION......................................................................................................... 1 1.1 Solid Oxide Fuel Cell ........................................................................................... 1 1.2 Glass Sealant ........................................................................................................ 2 1.3 Joint of Glass-Ceramic Sealant and Metallic Interconnect .................................. 5 1.4 Purposes and Scope .............................................................................................. 9 2. MATERIALS AND EXPERIMENTAL PROCEDURES........................................... 11 2.1 Mechanical Testing of Sintered GC-9 Glass ...................................................... 11 2.1.1 Materials and specimen preparation........................................................ 11 2.1.2 Ring-on-ring test ..................................................................................... 12 2.1.3 Weibull statistic analysis ......................................................................... 14 2.1.4 Microstructural analysis .......................................................................... 15 2.2 Mechanical Testing of Joint of Glass-Ceramic Sealant and Metallic Interconnect......................................................................................................... 15 2.2.1 Materials and specimen preparation........................................................ 15 2.2.2 Mechanical testing................................................................................... 17 2.2.3 Microstructural analysis .......................................................................... 17 3. RESULTS AND DISCUSSION.................................................................................. 19 3.1 Sintered GC-9 Glass ........................................................................................... 20 3.1.1 Microstructure ......................................................................................... 20 3.1.2 Effect of environmental temperature on mechanical behavior ............... 21 3.1.3 Fracture strength and Weibull statistic analysis ...................................... 22 3.1.4 Effect of environmental temperature on Young’s modulus..................... 24 VII 3.1.5 Failure analysis........................................................................................ 25 3.2 Joint of Glass-Ceramic Sealant and Metallic Interconnect ................................ 26 3.2.1 Effect of LSM coating on the joint strength............................................ 26 3.2.2 Creep rupture behavior............................................................................ 28 4. CONCLUSIONS......................................................................................................... 31 REFERENCES.................................................................................................................... 33 TABLES .............................................................................................................................. 37 FIGURES ............................................................................................................................ 39

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