臺灣博碩士論文加值系統

氫氣是一種理想乾淨的能源，而利用水分解產氫的方法，能使環境不受到汙染。然而，電解水反應需要一高效率的觸媒來降低反應所需的能量，至今，最有效的產氫觸媒依然是鉑，因此，尋找便宜、地球含量高的產氫觸媒是必要的，而硫化鉬已被證明為優秀的產氫觸媒。

本實驗利用低溫常壓熱解的方法來合成非晶相硫化鉬觸媒在碳紙基材上，然而，在前驅液乾燥過程中，液滴濕潤動態行為會影響硫化鉬形成不同的形態，因此，本實驗重點在於結合基材的親疏水性以及溶劑的極性，調整溶劑分子間的內聚力與溶劑和基材之間的附著力，藉以控制硫化鉬最後形成的形態。

將前驅物溶劑二甲基甲醯胺(DMF)和水混合且基材為親水碳紙，此結果具有相對較強的附著力，能夠使硫化鉬包覆著親水碳紙纖維，降低電荷傳導阻抗，讓電流密度在-0.20 V vs. RHE的電壓下增加到43 mA/cm2。因此，利用DMF和水的混合溶劑與親水碳紙成對可以合成出優秀的硫化鉬產氫觸媒。

Hydrogen is an ideal clean energy, and using the method of water splitting for hydrogen evolution reaction (HER), can prevent the environment from pollution. However, water splitting needs highly efficient catalysts to lower the overpotential. Till today, the most efficient catalyst for HER is still Pt. Therefore, finding a cheap and earth abundant catalyst for HER is essential. Molybdenum sulfide has been proved to be an excellent catalyst for HER.

In this study, the low temperature within atmospheric pressure for thermo-decomposition method to produce amorphous molybdenum sulfide (MoSx) catalyst on carbon paper substrates. However, during the precursor solution drying process, the dynamics of liquid wetting behavior dominates the morphology of MoSx. As a result, here, pairing the substrate hydrophobicity and solvent polarity, the cohesive force between solvent molecules and adhesive force between solvent and carbon paper substrates can be tuned, and thus the MoSx morphology can be controlled.

Pairing hydrophilic carbon paper with DMF+H2O mixing solvent results in a relatively strong adhesive force, it can make the well wrapped MoSx on carbon paper fiber structure. It can lower the charge transfer resistance and boost the current density to 43 mA/cm2 at -0.20 V vs. RHE. Therefore, using DMF+H2O mixing solvent and pair hydrophilic carbon paper can prepare the excellent MoSx catalyst for HER.

摘要I
AbstractII
致謝III
目錄IV
圖目錄VII
表目錄XII
第一章 緒論1
1.1 前言1
1.2 研究動機與目的1
第二章 文獻回顧3
2.1 氫能源3
2.2 氫氣的製備方法3
2.2.1石化燃料產氫3
2.2.2水分解產氫5
2.2.3生質能產氫7
2.3 電化學基礎理論與反應機制8
2.3.1電化學基本原理8
2.3.2電解水產氫8
2.3.3影響電解因素10
2.3.4極化與過電位11
2.3.5 Tafel方程式13
2.4 電解產氫之催化觸媒14
2.4.1常見之產氫觸媒14
2.4.2硫化鉬催化觸媒15
2.4.3提升硫化鉬催化效率之方法18
2.4.4非晶相硫化鉬22
2.5 界面現象23
2.5.1內聚力與附著力23
2.5.2親水性與疏水性24
2.5.3接觸角測量 24
第三章 實驗與分析方法27
3.1 實驗流程27
3.2 實驗儀器28
3.3 實驗藥品29
3.4 實驗步驟30
3.4.1疏水碳纖維基材前處理30
3.4.2親水碳纖維基材前處理31
3.4.3觸媒合成32
3.4.4電化學性質測試33
3.5 材料分析34
3.5.1電化學特性分析34
3.5.2場發射雙束型聚焦離子束顯微鏡 (Dual Beam Focused Ion Beam, FIB-SEM)40
3.5.3 X光繞射光譜儀 (X-ray Diffraction, XRD)41
3.5.4 X射線光電子能譜儀 (X-Ray Photoelectron Spectroscopy, XPS)42
3.5.5固著液滴影像數位化測量儀 (Video-image enhanced sessile drop tensiometer)43
4.1 電化學特性分析45
4.1.1線性掃描伏安法 (Linear Sweep Voltammetry, LSV)45
4.1.2電化學阻抗譜 (Electrochemical Impedance Spectroscopy, EIS)55
4.1.3電化學表面積 (Electrochemical Surface Area, ESA)57
4.1.4計時安培分析 (Chrono Amperometry)60
4.2 X光繞射圖譜分析 (XRD)61
4.3場發射雙束型聚焦離子束顯微鏡 (Dual Beam Focused Ion Beam, FIB-SEM) 62
4.3.1反應溫度62
4.3.2基材的親疏水性以及溶劑的極性64
4.4 X光電子能譜分析(X-Ray Photoelectron Spectroscopy, XPS)67
4.4.1反應溫度67
4.4.2基材的親疏水性以及溶劑的極性70
4.5 固著液滴影像數位化測量分析73
第五章 結論76
第六章 參考文獻77
附錄82

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