近年來，過度使用石化燃料造成了許多能源議題，包含能源的浩劫以及全球暖化所造成的氣候變遷與環境污染，這些議題逐漸地被受到注目，人們也進而尋求發展潔淨、高效能且具永續性之再生能源，以及發展產能與儲能相關應用的新技術來解決這些能源議題。為此目的，應用於染料敏化太陽能電池以及超級電容等等之綠能元件被認為是用來解決這些能源議題最佳的選擇。
本論文的第一部份我們以氧氣輔助低壓氣相沉積法發展了在透明導電基板上直接成長奈米碳管的技術，透過親水處理後並在此直接成長之奈米碳管表面利用電化學電鍍法分散二硫化鉬觸媒，建造成為一個具有三維立體之奈米複合結構，並做為染料敏化太陽能電池之對電極應用。而此直接成長之二硫化鉬/奈米碳管對電極應用於染料敏化太陽能電池具有約7.83 %的光電轉換效率，相對於傳統鉑金對電極而言，提升了將近10 %的光電轉換效率。我們的研究發現，二硫化鉬/奈米碳管這樣的一個三維立體奈米複合結構能夠完全取代鉑金的使用，並成為一個具有高效率、低成本的對電極材料應用於染料敏化太陽能電池。而在本論文的第二部分我們成功地製備了三維立體石墨烯結構，並在其表面直接成長奈米碳纖維成為一個具有高比表面積、低電阻且具有優異的縱向橫向電子傳導能力之三維立體複合電極，並應用於超級電容中。本論文的第三部分進一步的針對此複合碳材表面的親疏水性質做了更深入的探討，我們提供了一個快速親水的方式，透過酒精的浸泡處裡將疏水性的碳材表面轉換為親水性，更透過進一步的酸化處理來活化碳材表面的介孔/微孔結構增加固液介面的接觸面積，進一步提升了電極的電雙層電容量，而酸化處理所修飾的表面含氧官能基更提供了擬電容之儲能效果。這樣的一個活化過程提供了一個快速且簡單的方法，顯著的提升了元件之電容量以及能量密度。我們的研究將為未來高效率、低成本之染料敏化太陽能電池以及高能量密度之超級電容元件提供一個新的發展策略。

Recently, the issue of energy crisis were raised the attention of which looking for developing new, clean, efficient, and sustainable resources of renewable energy, as well as new technologies associated with energy conversion and storage. For this end, green energy applications for energy generation (DSSCs) and energy storage devices (Supercapacitors) have been promising candidates for the energy requirement.
In the first part of this thesis, we developed the directly synthesis of carbon nanotubes (CNTs) on FTO glass at low temperature via the low pressure chemical vapor deposition (LPCVD) method. The specimens were further underwent an electrochemical deposition process to decorate layed-MoS2 nano-catalyst and construct a 3D hybrid nanostructure as counter electrode (C.E.) materials for DSSCs. The DSSC assembled with MoS2/CNTs C.E. exhibiting the photoconversion efficiency value of 7.83 %, which was 9.5 % higher than that of the Pt film. Our findings demonstrated that the MoS2/CNTs hybrid nanostructure is a promising candidate for application as a highly efficient and low-cost C.E. material in Pt-free DSSCs. In the second part, we fabricated the full-carbon hybrid nanoarchitecture of carbon nanofibers/3D graphene (CNFs/3DG), this directly growth of binder-free CNFs/3DG hybrid nanoarchitecture provides strong adhesion to the substrate, low internal resistance, and excellently vertical and horizontal electron transmission ability for electron collection for supercapacitors application. In the third part, we provide an economic strategy of facile transition process of carbon nanomaterials surface from hydrophobic to hydrophilic by Ethanol-treatment process. Moreover, the CV-acid treatment further improve the ELDC by actived meso-/micro-pore structure at the electrode/electrolyte interface and introduced the pseudocapacitance by decorated surface oxygen-containing groups. This method remarkably enhanced the capacitance, energy density, and could be a promising candidate in high-performance supercapacitor applications.

Table of Contents
Abstract I
摘　要 II
誌　謝 III
Table of Contents V
List of Tables VIII
List of Figures IX
Chapter 1 Introduction 1
Chapter 2 Background and Theory 6
2.1. Dye-Sensitized Solar Cells (DSSCs) 6
2.1.1. Fundamental of DSSCs 7
2.1.2. Composition of DSSCs 9
2.1.2.1. Porous TiO2 Nanoparticles Working Electrode 9
2.1.2.2. Ruthenium (Ru)-Based Photosensitizer Dye 10
2.1.2.3. Electrolytes 12
2.1.2.4. Counter Electrode 13
2.1.3. The Characteristics of Solar Cells 14
2.2. Supercapacitors 15
2.2.1. Fundamental of Supercapacitors 15
2.2.1.1. EDLCs (Non-Faradaic process) 17
2.2.1.2. Pseudocapacitors (Faradaic process) 19
2.2.2. Test Configuration of Supercapacitors 19
2.2.3. The Characteristics of Supercapacitors 20
2.3. Carbon Nanomaterials 24
2.3.1. The Classical Carbon Nanomaterials 24
2.3.2. The Synthesis of Carbon Nanomaterials 26
2.3.3. Carbon Nanomaterials for Advanced Energy Conversion and Storage 28
2.3.3.1. Carbon Nanomaterials for Energy Conversion 29
2.3.3.2. Carbon Nanomaterials for Energy Storage 34
2.4. Molybdenum Disulfide 38
2.4.1. Ultrathin 2D Nanomaterials 38
2.4.2. The Typical Transition Metal Dichalcogenides (TMDs) Materials 39
2.4.3. The Synthesis of Molybdenum Disulfide 40
Chapter 3 Experimental Details 41
3.1. Electrochemical Deposition (ECD) and Analysis Systems 41
3.2. Oxygen-assisted Low Pressure Chemical Vapor Deposition (LPCVD) Systems 42
3.3. Sample Preparation 44
3.3.1. Part of DSSCs 44
3.3.2. Part of Supercapacitors 46
3.4. Instruments for Physical analyses, Photoconversion efficiency measurement and Electrochemical analysis. 47
Chapter 4 Hybrid Nanoarchitecture of Molybdenum Disulfide Anchored on Directly Grown Carbon Nanotubes (MoS2/CNTs) as a 3D Counter Electrode in Dye-sensitized Solar Cells 49
4.1. Low Temperature Direct Synthesis of MWCNTs on FTO glass 49
4.1.1. Introduction 49
4.1.2. Experimental 50
4.1.3. Results and Discussion 51
4.1.3.1. Investigation of FTO glass Thermal Degeneration 51
4.1.3.2. Oxygen Effect of the Directly Synthesis of MWCNTs on FTO glass 52
4.1.3.3. CNTs growth time vs. Length 53
4.2. Electrochemical Deposition of MoS2 on the Directly Grown MWCNTs as a 3D Counter Electrode in DSSCs 54
4.2.1. Introduction 54
4.2.2. Experimental 54
4.2.3. Results and Discussion 55
4.2.3.1. Composition and Morphologies 55
4.2.3.2. Electrocatalytic Properties 60
4.2.3.3. The Electrochemical Impedance Spectroscopy (EIS) properties 62
4.3. Charge-transfer speculated model 64
4.4. The Photovoltaic Performance of MoS2/CNTs Hybrid Counter Electrode in DSSCs 67
4.5. Conclusions 68
Chapter 5 Electrochemical Pulse Deposition of Ni Nanoparticles on the 3D Graphene to Synthesize CNFs as the Full-Carbon Hybrid Nanoarchitecture (CNFs/3DG) for Supercapacitors 70
5.1. Direct Synthesis of 3DG on Nickle Framework 70
5.1.1. Introduction 70
5.1.2. Experimental 71
5.1.3. Results and Discussion 72
5.2. Electrochemical Pulse Deposition of Ni Nanoparticles on the 3D Graphene to Synthesize CNFs/3DG Nanoarchitecture for Supercapacitors 75
5.2.1. Introduction 75
5.2.2. Experimental 76
5.2.3. Results and Discussion 77
5.2.3.1. Characterizations of CNFs/3DG hybrid electrode 77
5.2.3.2. Electrochemical Properties of CNFs/3DG hybrid electrode 80
5.3. Conclusions 83
Chapter 6 Hydrophilic Issue of Carbonaceous Nanomaterials and Further Functionalized Acid-treatment of CNFs/3DG Hybrid Nanoarchitecture for Supercapacitors 84
6.1. Hydrophilic Issue of Carbonaceous Nanomaterials 84
6.1.1. Introduction 84
6.1.2. Experimental 85
6.1.3. Results and Discussion 85
6.2. Functionalized Acid-treatment of CNFs/3DG Hybrid Nanoarchitecture for Supercapacitors 89
6.2.1. Introduction 89
6.2.2. Experimental 90
6.2.3. Results and Discussion 91
6.2.3.1. Characterizations of Functionalized-CNFs/3DG hybrid electrode 91
6.2.3.2. Electrochemical Properties of Functionalized-CNFs/3DG hybrid electrode 96
6.3. Charge-storage speculated model 100
6.4. Conclusions 101
Chapter 7 Summary and Outlook 102
Reference 108
Publication List 116

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