利用改變起始粉末晶面取向抑制 SrTiO3 第二相生成之研究

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研究生：	陳福強 Kevin Indrawan Sucipto
論文名稱：	利用改變起始粉末晶面取向抑制 SrTiO3 第二相生成之研究 Inhibition of second phase of interconnector by controlling surface orientation of SrTiO3 starting powder
指導教授：	施劭儒 Shao-Ju Shih
口試委員:	王丞浩 chen-hao wang 游進陽 Chin-Yang Yu 周育任 Yu-Jen Chou
學位類別：	碩士 Master
系所名稱：	工程學院 - 材料科學與工程系 Department of Materials Science and Engineering
論文出版年：	2019
畢業學年度：	107
語文別：	英文
論文頁數：	100
中文關鍵詞：	粉末、化學製備法、電子顯微鏡、鈣鈦礦
外文關鍵詞：	powders: chemical preparation
相關次數：	點閱：178 下載：3
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以鈦酸鍶作為固態氧化物燃料電池連接板之研究倍受關注，因其具有良好的化學及物理穩定性。然而，高溫退火處理形成之多晶樣品會發生相分離現象。第二相出現在具有較高鍶濃度的(100)平面，其源自於碳酸鍶的熱分解作用。
本研究之目的希望利用過氧化氫來控制SrTiO3¬晶體的表面能，達到降低{111}面族表面能，進而使{100}晶面減少。
研究中分別於前驅物中添加三個不同濃度 (0.03, 0.15, 和0.45M)的雙氧水，並利用噴霧熱裂解法製備鈦酸鍶粉末，再於1500ºC下進行燒結1小時、1000ºC下退火24小時，最後與未添加雙氧水的試片進行比較。
選擇使用噴霧熱裂解法製備是因為它簡單且能夠連續操作，具有高均勻的顆粒分佈結果。本研究合成之粉體部分利用X光繞射分析儀（XRD）、拉曼光譜儀、掃描式電子顯微鏡（SEM）、氮氣吸脫附分析儀（BET）分別鑒定相組成、表面形貌及比表面積。而燒結體則使用能量色散X-射線光譜（EDS）、XRD、阿基米德法分別進行相組成、表面形貌(元素組成)、相對密度。
最後由實驗結果得知，添加過氧化氫的多晶SrTiO3在1000℃ 24小時的熱處理下可以減少RP第二相的偏析。

Strontium titanate (SrTiO3)-based solid oxide fuel cell interconnectors have attracted more attention due to their chemical and physical stabilities. However, there is a phase segregation after become bulk specimen and annealed for period of time in high temperature. Second phase appeared on the Sr-rich (100) surface plane due to thermal decomposition of SrCO3. By controlling the crystalline SrTiO3 surface energy using hydrogen peroxide (H2O2), it can be lowering the {100} plane surface energy, so the population of {100} will be decreased. In this experiment, SrTiO3 powders were prepared by spray pyrolysis method using different concentration of H2O2 (0.03, 0.15, and 0.45M) and were sintered at 1500ºC for 1h and annealed at 1000ºC for 24h while comparing with un-treated sample. Spray pyrolysis was chosen because it is simple and able for continuous operation with high and uniform particles distribution result. As characterization, X-ray diffraction (XRD), Raman spectroscopy, and scanning electron microscopy (SEM) were conducted to research crystallographic phase and particle surface morphology. For bulk specimens, XRD, SEM-energy dispersive spectroscopy (EDS), Archimedes method, were conducted to research crystallographic phase, surface morphology, and relative density. Finally, H2O2-treated SrTiO3 bulk able to reduce the segregation of Ruddlesden Popper phase at 1000ºC for 24h.

CONTENTS
摘要        II
ABSTRACT        V
ACKNOWLEDGEMENTS    VI
CONTENTS        VII
LIST OF FIGURES    XI
LIST OF TABLES    XV
Chapter 1.    Introduction    1
1    Ceramic material    1
2    Strontium titanate second phase segregation    3
3    Purposes of this study    4
Chapter 2.    Literature review    6
1    Solid Oxide Fuel Cell    6
1.1    Solid Oxide Fuel Cell Interconnector part    8
2    Interconnector material    10
3    Properties of strontium titanate    11
3.1    Crystal structure of strontium titanate    12
3.2    Physical properties of strontium titanate    13
3.3    Surface energy of strontium titanate    13
4    Phase composition of strontium titanate    14
4.1    Ruddlesden-Popper (RP) phases    15
4.2    RP phase formation    16
5    Sintering    17
5.1    Stages of sintering    18
5.2    Sintering method    21
6    Spray pyrolysis    22
6.1    Ultrasonic spray pyrolysis equipment    22
6.2    Particle formation in the spray pyrolysis method    25
Chapter 3.    Experimental Procedure    28
1    Experimental materials    28
2    Experimental equipment    29
3    Preparation    31
3.1    Spray pyrolysis procedure    33
3.2    Die pressing and sintering    34
3.3    Annealing    34
4    Characterizations    35
4.1    X-ray diffraction    35
4.2    Nitrogen Adsorption/Desorption    35
4.3    Raman Spectroscopy    36
4.4    Field Emission Scanning Electron Microscope    37
4.5    Back-Scattered Electron Detector    39
4.6    Energy-dispersive X-ray Spectroscopy    40
4.7    Relative density    40
Chapter 4.    Results    42
1    SrTiO3 powders    42
1.1    Crystallographic phase    42
1.2    SrTiO3 powder particle surface morphology    44
1.3    Surface area    47
2    SrTiO3 bulk after sintering process    48
2.1    Crystallographic phase    48
2.2    Cross sectional micrograph    50
2.3    Relative density    52
3    SrTiO3 bulk after sintering and annealing process    53
3.1    Crystallographic phase    53
3.2    Scanning electron micrograph    55
3.3    Cross sectional micrograph    60
3.4    Relative density    62
Chapter 5.    Discussion    64
1    Influence of H2O2 to SrTiO3 particle shape    64
2    Influence of H2O2 to surface population.    65
3    SrTiO3 phase segregation    67
4    SrTiO3 bulk specimens’ grain    69
Chapter 6.    Conclusions    73
Chapter 7.    Future works    75
References        76


                                

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