臺灣博碩士論文加值系統

此篇論文著重在探索基本穩健且實用的光催化劑平台，以便在環境永續與可再生能源等具挑戰性的領域取得重大突破。為此我們開發了新穎智能光催化劑並建立其界面載子動力學與相關光催化活性的關聯性，包含典型的半導體/金屬異質結構光觸媒系統，ZnO/金屬（Au, Ag, Pd），特別是對於表面電漿共振誘導之界面載子動力學的定量分析。其中，ZnO-Au系統中對於等離子金屬含量，表面電漿共振誘導之載子傳遞，電場效應以及所量測到之電化學水分解反應中光活性提升間關聯性的建立為後續高效能且適當之電漿共振電化學水分解系統的開發提供確切實際的基礎。另外，我們還引進Ta, Nb, Zr等元素至TiO2奈米管中修飾其電子結構，並建立全空乏四元Ti−Nb−Ta−Zr−O (TNTZO)混合氧化物奈米管陣列，可作為後續建構複雜光電極系統所需之多樣化結構骨架。此外，通過顯著的載子分離和獨特過氧化氫酶特性之交互作用，可成功製備出具全天候活性之光催化劑- Au@Cu7S4修飾之TiO2奈米線。

This thesis focus on exploring essentially robust and practically efficient photocatalyst platform in order to make significant breakthrough to the ever-challenging fields of environmental sustainability and renewable energy. We developed the intelligent photocatalyst and demonstrated the correlations of their interfacial charge dynamics and photocatalytic activity including typical semiconductor/metal heterostructure photocatalyst system, ZnO/Metal (Ag, Au, Pd), especially for the quantitative analysis on the SPR-induced interfacial charge dynamics of ZnO-Au system. The correlations among plasmonic metal content, surface plasmon resonance-mediated charge transfer and electromagnetic response, and the resultant photoactivity enhancement toward photoelectrochemical (PEC) water splitting provide a solid foundation for creating effective and applicable plasmonic PEC cells. We also introduced Ta, Nb, Zr into TiO2 nanotube system to modify its electronic structures and established a fully depleted quaternary Ti−Nb−Ta−Zr−O (TNTZO) mixed-oxide nanotube arrays to serve as a versatile structural backbone for construction of a sophisticated photoelectrode paradigm. Besides, by coupling the pronounced charge separation and distinctive peroxidase mimic features, an all-day-active photocatalyst, Au@Cu7S4 nanocrystal-decorated TiO2 nanowires, were also successfully synthesized.

中文摘要 III
Abstract IV
Acknowledgement V
Table of Content VI
Chapter 1. Background and Motivation 1
Chapter 2. Metal-Particle-Decorated ZnO Nanocrystals: Photocatalysis and Charge Dynamicss 3
2.1 Introduction 3
2.2 Experimental Section 6
2.2.1 Preparation of PVP-Stabilized Metal Particles 6
2.2.2 Antisolvent Process for Metal-Decorated ZnO 6
2.2.3 Time-Resolved PL Analysis 7
2.2.4 Photocatalysis Experiment 7
2.2.5 Characterizations 8
2.3 Results and Discussion 9
2.4 Conclusions 21
2.5 References 22
Chapter 3. Plasmon-mediated charge dynamics and photoactivity enhancement for Au-decorated ZnO nanocrystals 28
3.1 Introduction 28
3.2 Experimental Section 31
3.2.1 Antisolvent process for ZnO–Au synthesis 31
3.2.2 Time-resolved PL measurements 31
3.2.3 PEC measurements 32
3.2.4 Electric field simulations 32
3.2.5 Characterization 33
3.3 Results and Discussion 34
3.4 Conclusion 51
3.5 Supporting Information 52
3.6 References 55
Chapter 4. Fully Depleted Ti−Nb−Ta−Zr−O Nanotubes: Interfacial Charge Dynamics and Solar Hydrogen Production 62
4.1 Introduction 62
4.2 Experimental Section 65
4.2.1 Anodization Growth of TNTZO 65
4.2.2 PEC Measurements. 65
4.2.3. Characterizations 66
4.3 Results and Discussion 68
4.4 Conclusions 85
4.5 References 86
Chapter 5. Au@Cu7S4 yolk@shell nanocrystal-decorated TiO2 nanowires as an all-day-active photocatalyst for environmental purification 92
5.1 Introduction 92
5.2 Experimental Section 95
5.2.1 Preparation of TiO2 nanowires 95
5.2.2. Decoration of Au particles 95
5.2.3. Further deposition of Cu2O and Cu7S4 95
5.2.4. Peroxidase-like activity measurement 96
5.2.5. Photocatalysis and dark-catalysis measurements 97
5.2.6. Characterizations 97
5.3 Results and Discussion 99
5.4 Conclusions 114
5.5 Supporting Information 115
5.6 References 118
Chapter 6. Summary and Outlook 124
Curriculum Vitae 126

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