臺灣博碩士論文加值系統

氫氣能源被視為未來重要的綠色能源之一，在許多的方法中，藉由光催化分解水產生氫氣更成為近年來熱門的研究議題。二氧化鈦等金屬氧化物更被廣泛地應用為光催化劑，然而較寬的能帶結構限制氧化物半導體的發展;相較於氧化物半導體，硫族金屬半導體有更合適的能帶結構以及優異的光學性質，被認為是有發展性的光催化材料。此篇論文提出如何增進光活性以及延長穩定性策略，並藉由時間解析螢光光譜分析載子動力學，進一步了解其效果提升背後的原因。而本論文分成三部分:
在第一部分當中，我們試著藉由更換硫族金屬半導體中的硫元素以及各成分元素的比例調整，進而控制半導體之能帶結構，將半導體的吸光範圍從可見光區域擴大至近紅外光區域，能有效地吸收入射光，並藉由材料表面的改質以及共催化劑的輔助之下，在所有的可見光波段中展現光活性，達到優秀的光催化產氫效率。在第二部分，則是藉由硫化物-二氧化鈦複合物異質半導體結構的設計，除了改善二氧化鈦對於可見光的吸收，並藉由異質結構的能隙平衡，增進光激發載子分離的效率，進而提升光催化反應，更最重要的是，在奈米柱狀二氧化鈦結構的幫助下，大大提升硫化物的光催化穩定性，提供一個全新的策略改善硫化物光腐蝕性的問題。
在最後的第三部分，則是整理並提出對於電化學水分解的未來趨勢，也列舉出具有潛力的材料，藉由能夠有效利用太陽光中紅外光區域之能量，期望未來能夠成為實際應用於綠色能源之方法。

Hydrogen energy is regarded as one of the important green energy. Among various methods, photocatalytic water splitting for hydrogen production becomes hot research project in recent years. Metal oxides such as titanium dioxide were widely utilized as photocatalysts, however, the wide band structures limit the progress of the metal oxides. Compared to metal oxide semiconductors, metal chalcogenide semiconductors which have proper band structures and excellent optical properties are considered as promising photocatalytic materials. In this thesis, the strategis for increasing photoactivities and prolonging stability were proposed. The reasons for improvement of photoactivities were further analyzed by time-resolved photoluminescence spectroscope. The thesis is classified into three parts:
In the first part, we tried control the band structure of semiconductor by replacing the sulfur element and adjusting the ratio of each elements in metal chalcogenide, so as to expand the absorption range from vibile region to infrared region. By surface modification and support of cocatalyst, it shows photoactivity in whole visible light region and exceptional hydrogen production efficiency. In the second part, by the design of sulfide-titanium dioxide heterostructure semiconductor, not only the absorption of titanium dioxide in visible light region is ameliorated but also the charge separation efficiency enhances through band alignment, and the performance of photocatalytic reaction therefore improves. Most importantly, with the support of nanorod-structure titanium dioxides, the photocatalytic stability of sulfide material shows superb improvement. It provides a noval strategy to modify the problem of photocorrosion for sulfide materials.
In the last third part, we organize and propose the future trend for the photoelectrochemical water splitting. We also list the potential materials for effectively utilizing the infrared light energy in sunlight, and expect that they have practical application to green energy.

摘要 I
Abstract II
誌謝 IV
Table of Content V
Figure Caption VII
Table Caption XII
Chapter 1. Background and Motivation 1
Chapter 2. Controlling Visible-Light Driven Photocatalytic Activity of Alloyed ZnSe-AgInSe2 Quantum Dots for Hydrogen Production 5
2.1 Introduction 5
2.2 Experimental Section 8
2.2.1 Chemicals 8
2.2.2 Preparation for ZAISe QDs 8
2.2.3 Surface modification with MPA 9
2.2.4 Photocatalytic H2 production 9
2.2.5 Characterizations 10
2.3 Results and Discussion 11
2.4 Conclusions 25
2.5 Acknowledgements 25
Chapter 3. TiO2 Nanowires-Supported Sulfides Hybrid Photocatalysts for Durable Solar Hydrogen Production 26
3.1 Introduction 26
3.2 Experimental Section 30
3.2.1 Chemicals 30
3.2.2 Preparation of TiO2 nanowires arrays 30
3.2.3 Chemical bath deposition of In2S3 and CdS 30
3.2.4 Characterizations 31
3.3 Results and Discussion 33
3.4 Conclusion 48
3.5 Acknowledgements 49
Chapter 4. Near Infrared-Driven Photoelectrochemical Water Splitting: Review and Future Prospects 50
4.1 Introduction 50
4.2 NIR-driven photoelectrodes 53
4.2.1 Chalcogenides 53
4.2.2 Chalcopyrites 58
4.2.3. Plasmonic metals 61
4.2.4. Plasmonic semiconductors 66
4.3 Outlook and perspectives 70
4.4 Acknowledgements 74
Chapter 5. Summary and Outlook 75
Reference 76

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