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研究生： Abiye Kebede Agegnehu
Abiye - Kebede Agegnehu
論文名稱： 二氧化鈦能隙調控工程與以低成本石墨烯為基礎之奈米複合材料於光催化水分解產氫之研究
Band Gap Engineering on Titania and Low Cost Graphene Based Nanocomposite Materials for Efficient Hydrogen Production via Photocatalytic Water Splitting.
指導教授： 黃炳照
Bing-Joe Hwang
蘇威年
Wei-Nien Su
口試委員: 周澤川
none
楊明長
none
林智汶
none
杜景順
none
周宏隆
Hung-Lung Chou
學位類別： 博士
Doctor
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2013
畢業學年度： 101
語文別： 英文
論文頁數： 182
中文關鍵詞： 光催化劑 、氧化石墨烯 、高度還原的氧化石墨烯 、納米粒子 、納米棒 、助催化劑 、氧化釩 、氧化
外文關鍵詞： highly reduced graphene oxide, vanadium oxide
相關次數： 點閱：445  下載：14 
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    • I have no Chinese abstract.

    A great technological challenge for H2 production from solar water splitting is the development of a clean and renewable energy carrier that does not utilize fossil fuels. One of the most attractive proposals is the large-scale utilization of hydrogen (H2) as a recyclable energy carrier. However, traditional industrial H2 production has limitations of consuming huge amounts of fossil fuels (e.g., natural gas), which results in equally large amounts of CO2 release. Photocatalytic and photoelectrochemical water splitting using semiconductor materials has thus attracted considerable interest due to its potential for clean production of H2 from water by utilizing abundant solar light. Thus the development of new efficient photocatalytic nanoarchitecture materials which are environmentally friendly, noble metal free, and visible region active is of paramount importance to tackle the current challenges of energy and environmental crisis.
    The main objective of this research has sought the practicality of solar to fuel conversion at a large scale. Thus the research focuses on investigation of multitalented nature of naturally abundant graphene based materials, and band gap engineering of the titanium dioxide towards visible region. The use of noble metal cocatalysts such as Pt has been completely avoided and rather low cost alternatives Ni, NiO, and highly reduced graphene oxide (HRGO) have been used as cocatalysts. Moreover, the well investigated titania based visible active photocatalyst has been prudently integrated with the newly discovered graphene based material for efficient hydrogen production from water splitting.
    Cocatalytic ultrafine Ni and NiO nanoparticles (2 to 3 nm diameter) were uniformly loaded on graphene oxide sheets using a simple chemical method. Water splitting activity from aqueous methanol solution under UV-visible light illumination was enhanced, approximately 4-fold for NiO/GO and 7-fold for Ni/GO, compared to bare GO. The highest activity (shown by Ni/GO) is attributed to the minimal electron-hole recombination resulting from the easy transfer of photogenerated electrons from the GO photocatalyst to the Ni cocatalyst. The relatively lower activity of NiO/GO may be due to the less efficient electron trapping ability of the NiO surface. A mechanism for the hydrogen gas evolution is proposed. This work revealed that a cocatalyst loaded on high surface area GO sheets can significantly enhance the evolution of hydrogen from aqueous methanol solution. This study offers a route to green energy harvesting using readily available low cost materials in combination with simple, versatile and scalable techniques. It also encourages the utilization of new graphene based materials which are adaptable to a wide variety of nanotechnology applications in many other areas.
    Moreover the band gap of titania is engineered by doping vanadium and the visible light responsive vanadium doped TiO2 nanoparticles (~ 6 nm diameter) have been successfully synthesized using a low temperature hydrothermal method. These nanoparticles were effectively composited with highly reduced graphene oxide (HRGO). Compared to undoped TiO2 nanoparticles and non-composited V-doped nanoparticles the nanocomposite exhibited enhanced hydrogen evolution under visible light illumination. The nanoparticles, loaded on HRGO, were intentionally fabricated as nanorods to enhance their contact with the HRGO sheets. Nanorod anchoring on HRGO, crystal structure, morphology and the porosity of the nanocomposite were analyzed by using EDX, XRD, TEM, and BET respectively. The photogenerated electrons were able to be trapped by the electron conducting HRGO sheet, thereby suppressing electron-hole recombination. For this reason, the nanocomposite material showed a better hydrogen evolution rate compared to the non-composited nanoparticles. This noble metal free nanocomposite material composed of highly conducting sheets loaded with stable, cheap and environmentally friendly titanium based porous nanorods also offers promise for other applications such as lithium ion batteries.

    Abstract ii Acknowledgment vi Table of Content vii List of Tables x List of Schemes xi List of Figures xii Chapter1 Introduction 1 1.1 Heterogeneous Photocatalysis and its Application 4 1.2 Fundamental principles and requirements of the photocatalysts 6 1.3 Evaluation of a photocatalytic water splitting efficiency 10 1.4 Varieties of photocatalyst materials for water splitting 12 1.4.1 Titanium oxide based semiconductor catalysts 13 1.4.2 Non-titania oxide photocatalysts 14 Chapter 2 Literature Review on Photocatalytysis and Solar to Fuel Conversion 16 2.1 Design and modification for nanomaterials for solar induced hydrogen evolution 16 2.2 UV-responsive photocatalysts for hydrogen production 17 2.2.1 d0 metal oxide photocatalysts 17 2.2.2 d10 metal oxide photocatalysts 22 2.2.3 f0 metal oxide photocatalysts 22 2.2.4 Nonoxide photocatalysts 23 2.2.5 Other new photocatalysts 26 2.3 Tailoring of visible light harvesting nanomaterials 29 2.3.1 Metal Ion doping 31 2.3.2 Nonmetal ion doping 33 2.3.3 Metal/nonmetal codoping 36 2.3.4 Creation of oxygen vacancies and oxygen sub stoichiometry 37 2.3.5 Dye sensitization 38 2.3.6 Semiconductor coupling 40 2.4 Approaches for efficient electron-hole separation 43 2.4.1 Noble metal cocatalyst loading 44 2.4.2 Metal oxide cocatalyst loading 47 2.4.3 Role of Sacrificial agents 51 2.5 Graphene based nanocomposite materials 53 2.6 Surface Plasmon effect 61 Chapter 3 Experimental and characterization 71 3.1 Experimental section 71 3.1.1 Chemicals 71 3.1.2 Preparation of GO 72 3.1.3 Preparation of Ni/GO and NiO/GO 72 3.1.4 Preparation of V-doped TiO2 nanospheres 73 3.1.5 Synthesis of V-doped TiO2/HRGO nanocomposite 73 3.2 Characterization 74 3.2.1 X-ray diffraction (XRD) analysis 74 3.2.2 Raman spectral analysis 75 3.2.3 Scanning electron microscopy and energy dispersive spectroscopy 76 analysis 76 3.2.4 Transmission electron microscopic analysis 77 3.2.5 Ultraviolet absorption analysis 78 3.2.6 Brunauer-Emmett-Teller (BET) analysis 79 3.2.7 X-ray photoelectron spectroscopy (XPS) analysis 80 3.2.8 X-ray absorption spectroscopy (XAS) analysis 81 3.2.9 Electrochemical measurements 82 3.2.10 Photocatalytic activity tests of GO, Ni/GO and NiO/GO 82 3.2.11 Photocatalytic activity tests of V- TiO2 and V-TiO2/HRGO 83 Chapter 4 Synthesis & Photocatalytic Application of GO, Ni/GO and NiO/GO 84 4.1 Motivation 84 4.2 Results and discussion 87 4.2.1 Oxidation of pristine graphite to graphene oxide 87 4.2.2 The formation of Ni and NiO on GO 91 4.2.3 Photocatalytic activities 95 4.2.4 Summary 99 Chapter 5 Synthesis of V doped TiO2 and its nanocomposite with HRGO 100 5.1 Motivation 100 5.2 Results and Discussion 102 5.2.1 Doping of V into TiO2 102 5.2.2 Growth Mechanism of V-TiO2 nanorods on HRGO surface 115 5.2.3 Photocatalytic activity 116 5.3 Summary 122 Chapter 6 Conclusions 123 Chapter 7 Future Outlook 126 References 131 Curriculum Vitae of Author 143 List of research papers 144 Conference/Workshop presentations 145

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