本論文致力於研究鋰離子電池之陽極材料。
自索尼公司26年前（1991年）宣布推出一種名為鋰離子電池的全新儲能設備以來，電池研究得到了廣泛的發展。由於重量輕，能量密度高，循環穩定性好，鋰離子電池可用於各種便攜式設備和電動汽車（EV），混合動力電動汽車（HEV）和插電式電動汽車（PEV）。研究人員積極研究低成本，高存儲容量和更安全的電極材料。目前為止，石墨是最廣泛使用的商業陽極材料，其機制為嵌入性陽極材料，但其低理論容量（372 mA h g-1）限制了在高能量密度要求中的應用。鋰鈦氧化物為另一種嵌入性商業化材料，具有優異的循環壽命和低時間消耗，但具有低容量（< 200mA h g-1）和高電阻率。矽基和過渡金屬氧化物基轉換材料的容量超過1000 mA h g-1，但在充電/放電過程中嚴重的體積變化會導致嚴重的容量遞減，一般多使用奈米碳管或石磨烯以及製作複合材料改良這些問題。
1985年發現的C60（富勒烯）拓展了人類對高度對稱分子化學的新視野。本論文中主要探討Mo-V和Mo-Fe混合的Keplerate多金屬氧酸鹽（POMs），一種類富勒烯金屬氧化物，其合成方法為相對簡單的溶液法，可大幅節省製程成本。由於Mo，V和Fe的各種氧化態（Mo2 + ~Mo6 +，Fe2 + ~Fe8 / 3 +和V2 + ~V5 +），在充放電過程中Mo-V和Mo-Fe混合POM中的多個氧化還原中心導致高電容量和優異的穩定性，並且無需任何輔助添加劑和碳質材料，即可達到優越的性質。

Abstract
This dissertation focuses on the anode materials of lithium-ion batteries (LIBs).
Research in batteries has widely developed since Sony Corporation announced a brand-new energy storage device called lithium-ion battery 26 years ago (1991). Because of the light weight, outstanding energy density, and well cycling stability, LIBs are up to grade for a wide range of portable devices and electric vehicles (EV), hybrid electric vehicles (HEV) and plug-in electric vehicles (PEV). Researchers have aggressively studied lower-cost, higher-storage capacity, and safer electrode materials. Graphite is the most widely used commercial anode material, but its low theoretical capacity (372 mA h g-1) restricts the application in high energy density demands. Lithium-titanium–based Li-insertion materials possess excellent cycle life and low-time-consuming yet suffer from low capacity (< 200 mA h g-1) and high electrical resistivity. Silicon-based and transition-metal-oxide-based conversion materials owe over 1000 mA h g-1 capacity, but severe volume changes during charging/discharging processes leads to vicious capacity fading.
The discovery of C60, as known as fullerene, in 1985 have brought us to a new horizon in the chemistry of highly symmetric molecules. Herein, we report Mo-V and Mo-Fe-mixed Keplerate polyoxometalates (POMs), a kind of Fullerene-like metal oxide clusters, which was synthesized through a simple solution process as anode material for LIBs. Because of diverse oxidation states of Mo, V, and Fe (Mo2+~Mo6+, Fe2+~Fe8/3+ and V2+~V5+), the multiple redox centers within Mo-V and Mo-Fe mixed POMs during charge-discharge processes result in high capacity and excellent stability individually without any supporting additives and carbonaceous materials.

Table of Contents I
List of Tables IV
List of Figures V
Chapter 1. Introduction 1
1.1 Background and Motivation 1
1.2 Dissertation Overview 6
Chapter 2. Literature Review 7
2.1 Lithium-Ion Batteries (LIBs) 7
2.1.1 Basic Principles of LIBs 10
2.2 Anode Materials for Lithium-ion Batteries 10
2.2.1 Overview of Anode Materials 10
2.2.2 Insertion Materials 13
2.2.3 Alloying Materials 15
2.2.4 Conversion Materials 16
2.3 Anode Materials for Sodium-ion Batteries 19
2.3.1 Basic Principle of NIBs 19
2.3.2 Insertion Materials 20
2.3.3 Alloying Materials 22
2.3.4 Conversion Materials 23
2.4 Polyoxometalates (POMs) Anode Materials 24
2.4.1 The Research Scopes of POM Anodes in This Thesis 28
Chapter 3. Experimental Methodology 30
3.1 Synthesis and Characterization of {Mo72V30} 30
3.1.1 Synthesis of {Mo72V30} 30
3.1.2 Material Characterization of {Mo72V30} 31
3.2 Synthesis and Characterization of {Mo72Fe30} 33
3.2.1 Synthesis of {Mo72Fe30} 33
3.2.2 Material Characterization of {Mo72Fe30} 34
3.3 Half Cell Preparation and Electrical Characterization 35
3.3.1 Electrode Preparation 35
3.3.2 LIB Half-cell Configuration 35
3.3.3 NIB Half-cell Configuration 36
3.3.4 Electrochemical Characterization Methods 36
3.4 LIB Full Cell Preparation 39
Chapter 4. Result and Discussion 40
4.1 Materials Characterization 40
4.1.1 Material Characterization of {Mo72V30} 40
4.1.2 Material Characterization of {Mo72Fe30} 49
4.2 Electrical Characterization of {Mo72V30} 55
4.2.1 Electrical Characterization of {Mo72V30} in LIBs 55
4.2.2 Electrical Characterization of {Mo72V30} in NIBs 71
4.2.3 Full Cell Study of {Mo72V30} LIB 76
4.3 Electrochemical Characterization of {Mo72Fe30} 78
4.3.1 Electrochemical Characterization of {Mo72Fe30} in LIBs 78
4.4 Summary of Chapter 4 84
Chapter 5. Conclusion 86
Chapter 6. Future Works 89
Publications 91
Awards 92
Conference 92
References 93

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