臺灣博碩士論文加值系統

碲化鉍（Bi2Te3）是一種在室溫環境下具有良好熱電性能熱電材料，並且在發電的過程不會造成污染。熱電效率由熱電優值(Thermoelectric figure of merit) ZT 來評估，透過開發優質熱電元件增加ZT值是有效提來高轉換效率的方法之一。在本研究中，我們使用分子動力學來研究具有不同效應的Bi2Te3和BixSb2-xTe3化合物五重層奈米薄膜的機械和熱導率特性。結果表明，Bi2Te3奈米薄膜在機械特性在完美無缺陷結構的奈米薄膜具有理想的楊氏模數，並且表現出很強的溫度依賴性，而具有界面缺陷時，原子排列的結構紊亂影響了機械性能；在熱傳導特性，聲子遇到晶格無序的原子區會產生散射而降低熱傳導，具有Te界面會引起強聲子散射，並驗證奈米尺度下具有結構自我修復機制，傳遞熱通量時會經歷自我修復過程提高熱導率，奈米膜中的界面缺陷會影響熱導率和界面熱阻。此外，摻雜不同比例Sb元素的BixSb2-xTe3化合物奈米膜影響其機械和熱導率特性，並與純Bi2Te3奈米膜有很大差異，BixSb2-xTe3化合物奈米膜比純Bi2Te3奈米膜表現出更好的機械拉伸強度，熱傳導時產生SbTe反位缺陷並改變熱導率。最後，我們使用區熔法製備了Bi2Te3奈米結構，並透過奈米壓痕和即時動態穿透式電子顯微鏡研究壓縮載荷下的機械性能，結果表明，在高載荷條件下，材料結構中存在多種錯位和相變，力-位移曲線會觀察到明顯的“突進”現象，而彈性模數分別透過奈米壓痕系統與即時動態壓縮系統測量為42.7±2.56 GPa與12.3±0.1 GPa。這項研究的成果，有助於Bi2Te3和BixSb2-xTe3化合物的熱電元件開發的優化與應用。

Bismuth telluride (Bi2Te3) is a type of thermoelectric (TE) material used for energy generation that does not cause pollution. Increasing the thermoelectric figure of merit (ZT) which can represent the conversion efficiency of TE materials is one of the most important steps in the development of thermoelectric components. In this study, we use molecular dynamics to investigate the thermal conductivity and mechanical properties of quintuple layers of Bi2Te3 and BixSb2-xTe3 nanofilms with different effects. The results indicate that the Bi2Te3 nanofilm perfect substrate has the ideal Young’s modulus and thermal conductivity and show a strong temperature dependence of the thermal conductivity for Bi2Te3 nanofilms with an ideal structure. As the interface changed, the structural disorder of atomic arrangement affected the mechanical properties; moreover, the phonons encounter lattice disordered atomic region will produce scattering reduce heat conduction. We also verified the self-assembly mechanism for nanoscale Bi2Te3 and found that the Bi2Te3–Te interface induces strong phonon scattering. Thus, interfacial defects in Bi2Te3 nanofilms affect the thermal conductivity and the thermal boundary resistance (TBR). In addition, BixSb2-xTe3 nanofilms are significantly affected by Sb content and differ greatly from those of pure Bi2Te3 nanofilms. Furthermore, BixSb2-xTe3 nanofilms exhibit better tensile strength than pure Bi2Te3 nanofilms. Changes in Sb content strongly affect the concentration of SbTe antisite defects and alter thermal conductivity. Finally, we prepared Bi2Te3 nanostructures via zone melting (ZM) and characterized their mechanical properties by nanoindentation and in situ transmission electron microscopy (TEM). The nanoindentation results revealed that a significant ‘pop-in’ phenomenon occurs under high-loading conditions with multiple dislocations and phase transitions in the material structure. Young’s modulus of the nanostructures was found to be 42.7 ± 2.56 GPa from nanoindentation measurements and 12.3 ± 0.1 GPa from in situ TEM measurements. The results of this study may be useful for optimizing Bi2Te3 and BixSb2-xTe3 thermoelectric devices in the future.

摘 要 i
Abstract ii
誌 謝 iv
Contents v
List of table captions vii
List of figure captions viii
Symbol table xii
Chapter 1 Introduction 1
1.1 Background 1
1.2 Thermoelectric materials 3
1.3 Motivation 6
1.4 Thesis organization 8
Chapter 2 Literature review 9
2.1 Literature review of Molecular Dynamics 9
2.1.1 Basic theory of Molecular Dynamics 9
2.1.2 Interatomic force and Potential energy function 11
2.1.3 Thermal characteristic simulation 15
2.2 Literature review of Bismuth telluride 17
2.2.1 Materials and potential energy function 19
2.2.2 Determination of thermal and mechanical properties 22
Chapter 3 Materials and method 25
3.1 Simulation method 25
3.2 Experimental method 31
3.2.1 Preparation of the material 32
3.2.2 Measurement devices 34
Chapter 4 Results and Discussion 43
4.1 Prediction of thermal conductivity and mechanical properties of Bi2Te3 nanofilms 43
4.1.1 Effects of interfacial defect on thermal conduction 44
4.1.2 Effects of atomic arrangement structure on mechanical property 58
4.2 Prediction of thermal conductivity and mechanical properties of Bi-Sb-Te nanofilms 67
4.3 In situ deformation and mechanical properties of Bi2Te3 prepared via zone melting 80
4.3.1 Morphology and surface microstructure 81
4.3.2 Mechanical properties measured 83
Chapter 5 Conclusions 88
Acknowledgements 91
References 92
Curriculum vitae 102
Publication list 103

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