此研究致力於研究與開發熱力學平衡之材料系統應用於SOFC連接板。採用低熱膨脹係數超合金 HRA929作為基板，根據CALPHAD-based模擬軟體JMatPro所模擬之800°C平衡相圖來設計保護塗層成份。靶材與塗層成份之試片皆由真空電弧熔煉(VAM)製備，並鍍覆1 m的薄膜於HRA929上。利用恆溫氧化實驗來觀察塗層成份試片的氧化層成長情形並觀察塗層與基材間的交互擴散。材料系統的面積比電阻(ASR)使用四線量測法。塗層成份的熱膨脹係數是利用TMA量測而得。
由實驗結果得知本研究所研發的材料系統(coating 4+ HRA929)之抗氧化能力與面積比電阻表現具有商業化材料之水準，且塗層與基材間的熱膨脹表現相近。由鍍覆coating 4之HRA929試片，於800 °C下退火100小時，發現塗層與基材界面穩定且交互擴散情形很低(塗層與基材達到近熱力學平衡)，可提升作為SOFC連接板之使用壽命。再者，此材料系統與LSM層的界面匹配性良好，且可生成錳鉻尖晶石抑制Cr向外擴散。

The present study focuses on developing a materials system for the SOFC interconnect application. This study has utilized a low thermal expansion material HRA929 as the substrate and designed a coating composition based on CALPHAD-based phase diagram simulation at 800°C. The ingots of coating compositions were prepared by vacuum arc melting (VAM); coating process was magnetron sputtering, and a 1 m thin film of the coating was deposited on the surface of HRA929. Isothermal oxidation tests were conducted to observe the growth of oxide scale and interdiffusion between coating and substrate. Four-wire method was employed to measure the high temperature area specific resistance (ASR) of the system. Thermal mechanical analysis was performed to measure the coefficient of thermal expansion (CTE). The ASR performance and oxidation resistibility of our materials system were comparable to commercialized material, while the CTE of coating and substrate was similar. The phase stability of the interface between coating and substrate was stable after 100 hours exposure at 800°C. Moreover, this materials system exhibited phase stability at the interface and interdiffusion was minimized, hence the life of acting as interconnect can be prolonged. Furthermore, the compatibility of coating and LSM was good and the formation of (Mn,Cr)3O4 can suppress the outward diffusion of Cr.

Abstract I
摘要 II
Acknowledge III
Table of Contents VII
List of Figures X
List of Tables XV
I. Introduction 1
II. Literature Review 3
2.1 Fuel Cells 3
2.2 Solid oxide fuel cells (SOFCs) 5
2.2.1 Advantages of SOFC 6
2.2.2 Electrolyte 7
2.2.3 Anode 7
2.2.4 Cathode 8
2.2.5 Interconnect 8
2.3 Protective coatings for interconnect 10
2.3.1 Rare earth perovskite coatings 10
2.3.2 Spinel coatings 11
2.4 Area Specific Resistance (ASR) 14
2.5 HRA929 15
2.6 Bond coat 17
2.7 Coating composition design tools - Jmatpro and Thermocalc 19
III. Materials and Methods 20
3.1 Material selection and coating design 20
3.2 Experimental procedure 24
3.3 Aging 25
3.4 Heat treatment 25
3.5 X-ray Diffractometer 28
3.6 SEM 28
3.7 Coefficient of thermal expansion (CTE) 28
3.8 Oxidation test 29
3.8.1 Oxidation weight gain test 29
3.8.2 Oxide scale observation 29
3.9 Area Specific Resistance (ASR) 29
3.10 Target preparation 30
3.11 Coating deposition 30
3.12 Interface stability and phase stability 31
IV. Results and Discussion 32
4.1 Thermodynamic equilibrium microstructure of HRA929 at 800 C 32
4.2 Coating materials – Intrinsic properties 38
4.2.1 Isothermal oxidation tests 38
4.2.2 Oxide scale analysis 42
4.2.3 Coefficient of thermal expansion 49
4.2.4 ASR 52
4.3 Coating compatibility and interface stability with substrate 54
4.4 Coating compatibility with LSM 58
4.5 Microstructure evolution of coating 4 63
V. Conclusions 70
VI. Future Work 71
VII. References 72

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