本研究於奈米碳管電沉積特殊形貌白金觸媒並應用於甲醇燃料電池陽極，先以熱化學氣相沉積奈米碳管於碳紙上，再以電鍍合成白金於奈米碳管上，探討不同型貌白金之觸媒特性。藉由奈米碳管增加表面積使白金分布更佳及尋求活性最佳的白金結構，降低甲醇燃料電池觸媒之價格，使甲醇燃料電池的價格降低，進而使其更能有商用化發展。
奈米碳管藉由化學沉積法直接成長於碳紙上以增加電極表面積，經由親水處理後，再以不同電位電沉積白金，亦製備商用觸媒以作為對照組。分析方面，使用掃描式電子顯微鏡(SEM), 穿透式電子顯微鏡(TEM), X光繞射儀 (XRD), 及感應耦合電漿質譜分析儀 (ICP-MS) 做表面特性結構分析。白金電子結構使用高解析電子能譜儀分析(HRXPS)。 從SEM及TEM結果顯示，隨著電位越負，金屬還原後形貌從球狀逐漸變成鈍角、樹枝狀、片狀結構。而從高解析穿透式電子顯微鏡及X光繞射儀等表面分析亦可得到樹枝狀結構白金原子排列最整齊，因此透過CHI1140B電化學分析儀進行循環伏安法測試甲醇氧化反應結果，奈米樹枝結構之白金確實具較高的催化甲醇氧化表面活性，高於商用觸媒 3.67倍。而奈米片狀結構之白金觸媒因其具有最高的表面積與體積比(S/V ratio)，因此可以較少量的白金給予較高的表面積，因此其具最高的質量活性，高於商用白金2.95倍。

In this study, we herein suggest synthesizing four different morphologies of Pt onto Carbon nanotubes (CNTs) / Carbon paper (CP) by the electrodeposition method as an electrocatalyst with the higher activity for methanol oxidation to increase the performance of DMFCs. Scanning Electron Microscope (SEM), Transmission Electron Microscopy (TEM), X-ray diffraction (XRD), and Inductively coupled plasma mass spectrometry (ICP-MS) were employed to study the morphological and structural features of Pt/ CNTs /CP. The electronic structures of Pt were examined by X-ray photoelectron spectroscopy (XPS). All electrochemical measurements were carried out with a CHI1140B Potentiostat and examined by Cyclic Voltammetry method (CV). The electrocatalytic activity of prepared electrodes was determined by the mass activity (MA) and surface activity (SA) for the methanol oxidation reaction. For nano dendrite-like of Pt, the catalyst specific activity (SA) for the methanol oxidation reaction is 3.67 times better than that of a commercial Pt-black catalyst, and for nanosheet-like of Pt, the mass activity (MA) value is 2.95 times higher than that for Pt-black.

Abstract i
摘要 ii
致謝 iii
Table of Content v
List of Tables viii
List of Figures ix
Chapter 1. Introduction 1
Chapter 2. Literature Reviews 4
2.1 Fuel Cells 4
2.2 Fundamentals of Direct Methanol Fuel Cell 8
2.2.1 The working principle of DMFC 8
2.2.2 Composition of DMFC 9
2.3 Platinum (Pt) 12
2.3.1 The properties of Pt 13
2.3.2 Various morphologies of Pt 14
2.3.4 Methanol oxidation mechanism of Pt 23
2.4 Supporting materials for catalyst 25
2.4.1 Conductive polymers 25
2.4.2 Carbon nanomaterials 26
2.4.3 Synthesis of Pt/ CNTs by electrochemical deposition method 31
2.5 Preparation methods of catalyst 32
2.5.1 Impregnation method 32
2.5.2 Colloidal method 33
2.5.3 Microemulsion method 33
2.5.4 Electrochemical deposition method 34
Chapter 3. Experiment details 36
3.1 Experiment Process 36
3.2 Chemicals and Instruments 38
3.2.1 Chemicals 38
3.2.2 Gas 38
3.2.3 Experiment Instruments 38
3.2.4 Analysis Instruments 39
3.2.5 Three-electrode electrochemical system 40
3.3 Synthesis of CNTs by thermal chemical vapor deposition 41
3.4 Hydrophilic treatment of CNTs and deposition of Platinum 42
3.5 Deposition of Platinum 42
3.6 Electrochemical analysis 42
3.7 Characterization and instruments 43
Chapter 4. Result and discussions 49
4.1 Carbon nanotubes (CNTs) 49
4.1.1 The CNTs prepared at different temperature 49
4.1.2 The CNTs prepared at 850 ºC 54
4.1.3 The hydrophilic treatment of the CNTs 55
4.2 Pt deposited on CNTs 56
4.2.1 Morphology Characterization 56
4.2.2 XRD results 60
4.2.3 XPS results 62
4.2.4 Electrochemical test 65
Chapter 5. Conclusions 68
References 69

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