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研究生： 林彥蓁
論文名稱： 利用X光吸收光譜分析燃料電池陰陽極觸媒FexPt1-x與Fe1-xPtRux之表面組成與電催化特性
指導教授： 陳家俊
學位類別： 碩士
Master
系所名稱： 化學系
Department of Chemistry
論文出版年： 2008
畢業學年度： 96
語文別： 中文
中文關鍵詞： 燃料電池 、陰陽極觸媒 、x光吸收光譜
論文種類： 學術論文
相關次數： 點閱：188  下載：0 
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    • 本篇旨在研究兩元及三元觸媒結構與電催化活性的關係。作為陰極觸媒之FePt是一種比單純Pt具較高氧氣還原反應活性之合金，而作為陽極觸媒之FePtRu，其主要是用於測是對CO剝除與甲醇催化的效果。利用XAS中的EXAFS數據分析結構及表面組成，並觀察其以旋轉電極測試之CO剝除、甲醇催化與氧氣還原反應的影響。FePt系列與FePtRu系列樣品粒徑大小皆約為3-5 nm，關於這兩系列研究所用到的儀器與分析主要為XRD、TEM與XAS。

    陰極催化方面，在FePt系列觸媒中以FePt11具有最好的氧氣還原活性，根據文獻與表面組成，發現FePt11具有最適當的5d空軌域有助於氧氣還原。另外在陽極催化方面，以FePtRu 10hr催化能力最好，推測其表面組成最接近一比一比一，電子間提供-接受達平衡，因此表現最好。

    目錄 總目錄...............................................................................................................Ⅰ 中文摘要...........................................................................................................Ⅳ 英文摘要...........................................................................................................Ⅴ 第一章 緒論.......................................................................................................1 1.1 前言..............................................................................................................1 1.2 燃料電池簡介..............................................................................................2 1.2.1 燃料電池的種類...............................................................................4 1.2.2 燃料電池內的電化學反應...............................................................5 1.3 直接甲醇燃料電池( Direct methanol fuel cell )發展..................................9 1.3.1 DMFC陽極觸媒..............................................................................10 1.3.2 DMFC電解質..................................................................................13 1.3.3 DMFC陰極材料..............................................................................14 1.4 研究動機與方法........................................................................................20 第二章 原理.....................................................................................................21 2.1 X光吸收光譜原理..............................................................................21 2.1.1 X光吸收近邊緣結構 (XANES).....................................................21 2.1.2延伸X光吸收微細結構 (EXAFS).................................................23 2.1.3 數據分析.........................................................................................27 2.2 粉末X光繞射光譜(Powder X-ray Diffration)...........................................32 2.3穿透式電子顯微鏡(Transmission electron Microscopy)...........................34 2.4 電化學原理................................................................................................36 2.4.1 循環伏安法.....................................................................................36 2.4.2 極化曲線.........................................................................................40 2.4.3 旋轉盤電極(Rotating Disc Electrode, RDE).................................41 第三章 實驗部份.............................................................................................44 3.1 實驗藥品及設備........................................................................................44 3.1.1 實驗藥品.........................................................................................44 3.1.2 實驗設備.........................................................................................46 3.2 樣品合成....................................................................................................47 3.2.1碳黑之前處理..................................................................................47 3.2.2 合成FePt奈米粒子.........................................................................48 3.2.3 合成FePtRu奈米粒子....................................................................48 3.2.4 觸媒製備.........................................................................................49 3.3 材料鑑定與分析........................................................................................49 3.3.1 XRD分析.........................................................................................49 3.3.2 TEM分析.........................................................................................50 3.4 電化學特性測試........................................................................................50 3.4.1 電極之清洗...................................................................................51 3.4.2電極片製備.....................................................................................52 3.4.3電化學特性量測.............................................................................52 3.4.3.1 循環伏安..........................................................................53 3.4.3.2 CO剝除測試.....................................................................53 3.4.3.3 甲醇氧化極化曲線..........................................................53 3.4.3.4 氧氣還原測試..................................................................53 3.5 X光吸收光譜(XAS)................................................................................54 3.5.1 EXAFS之曲線適配.........................................................................54 3.5.2 以X光吸收光譜分析觸媒結構.....................................................55 第四章 結果與討論..........................................................................................59 4.1 陰極觸媒材料.............................................................................................59 4.1.1 合成FePt奈米粒子........................................................................59 4.1.2 材料之晶相與形態分析.................................................................60 4.1.3 XANES之吸收係數.....................................................................64 4.1.4 X光吸收光譜...............................................................................64 4.1.4.1 X光吸收近邊緣結構(XANES).......................................64 4.1.4.2 延伸X光吸收微細結構(EXAFS)....................................66 4.1.5 觸媒材料之結構比較.....................................................................70 4.1.6 電化學特性量測結果.....................................................................72 4.1.6.1 循環伏安法........................................................................72 4.1.6.2 線性掃描伏安法................................................................74 4.1.7 陰極觸媒電化學活性之比較.........................................................76 4.2 陽極觸媒材料.............................................................................................77 4.2.1 合成FePtRu奈米粒子...................................................................77 4.2.2 材料之晶相與形態分析.................................................................77 4.2.3 XANES之吸收係數.....................................................................80 4.2.4 X光吸收光譜...............................................................................80 4.2.4.1 X光吸收近邊緣結構(XANES)..........................................80 4.2.4.2延伸X光吸收微細結構(EXAFS)......................................83 4.2.5觸媒材料之結構比較.......................................................................88 4.2.6 電化學特性量測結果.....................................................................90 4.2.6.1 循環伏安法........................................................................90 4.2.6.2 線性掃描伏安法................................................................93 4.2.6.3 CO剝除...............................................................................94 4.2.6.4 甲醇氧化極化曲線............................................................96 4.2.7 陽極觸媒材料之電化學活性比較.................................................98 第五章 結論...................................................................................................101 5.1 結論..........................................................................................................101 5.2 未來展望..................................................................................................102 第六章 參考資料...........................................................................................102

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