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研究生: 林家正
Chia-Cheng Lin
論文名稱: 中孔洞二氧化矽、金屬與高分子之共嵌入化學
The Incoporatons of Metal and Polypyrrole into mesoporous silica
指導教授: 楊家銘
Chia-Min Yang
口試委員:
學位類別: 碩士
Master
系所名稱: 理學院 - 化學系
Department of Chemistry
論文出版年: 2006
畢業學年度: 94
語文別: 英文
論文頁數: 162
中文關鍵詞: 中孔洞二氧化矽鉑釕直接甲醇燃料電池聚吡咯
外文關鍵詞: SBA-15, PtRu, DMFC, polypyrrole
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  •   本研究內容,主要探討中孔洞二氧化矽、金屬與高分子之共嵌入化學。中孔洞二氧化矽(SBA-15)為一具有高表面積以及規則孔洞排列之奈米結構,可應用於觸媒以及其他許多方面上。
      在第一部分,研究利用SBA-15作為模板與鐵及聚吡咯的複合系統中,聚吡咯高溫裂解的過程中鐵之化學環境之變化。而在第二部分之中,則研究白金釕雙金屬與聚吡咯及SBA-15三者的複合系統。在直接甲醇燃料電池上,對於一氧化碳的毒化問題,白金釕雙金屬系統是很重要的陽極觸媒。聚吡咯則是一具有導電性質的導電高分子。利用SBA-15提供空間的侷限下,藉由控制實驗條件以期能得到不同奈米結構金屬粒子與聚吡咯之複合材料。
      在X光吸收光譜的分析下,隨著各個處理過程,鐵的化學環境變化被細部地觀察與探討。白金釕雙金屬之奈米結構可藉由不同實驗條件控制為個別金屬粒子或核殼結構等。電化學活性與金屬結構之關係則待更進一步的實驗量測。


    In this thesis, the co-incorporation of metal and polypyrrole into mesoporous silica was studied. Mesoporous silica possesses high surface area and ordered pore structure that enables the applications in catalysis, separation and so on. The employment of vapor-phase oxidative polymerization of PPY as carbon precursor possesses the stoichiometric relationship enables the rational control of carbon loading. In part I, the evolution of the chemical environment of iron during the pyrolysis process was investigated by X-ray absorption spectroscopy. In part II, extending the work of part I, the corporation of electrocatalyst, i.e. PtRu, and PPY is investigated. PtRu is considered the best anode catalyst toward the poison of CO. Several PPY/PtRu/SBA-15 composites are designed and performed for the anode materials of DMFC. The preliminary result from XAS suggests that the alloy structure of PtRu particles could be controlled as core-shell or separate particles by tuning the experimental parameters. The further electrochemical analysis is in progress.

    Contents Chapter 1. Introduction 1-1 Mesoporous materials 1-2 Inclusion chemistry of Mesoporous silica 1-2-1 The inclusion of polypyrrole 1-3 DMFC and the PtRu system 1-4 systems studied in this thesis Chapter 2.Experimental and characterization sections 2-1 Chemicals 2-2 The preparation of Fe/PPY/SBA-15 composite 2-2-1 The synthesis of SBA-15 2-2-2 The incorporation of iron salt 2-2-3 The pyrrole vapor treatment 2-2-4 The experimental procedure 2-3 The preparations of PtRu/PPY/SBA-15 composites 2-3-1 The synthesis of supports 2-3-2 Sodium borohydride (SBH) treatment 2-3-3 The Pt prior series I and II 2-3-4 The Ru prior series I, II and III 2-3-5 The simultaneous PtRu series I and II 2-3-6 The single metal series 2-4 Characterizations 2-4-1 X-ray Absorption spectroscopy 2-4-2 The XAS measurement 2-4-3 PXRD 2-4-4 The Cyclic voltammetry 2-5 The summary of the notations Chapter 3. Results and discussions 3-1 The silica/Fe/PPY composites 3-1-1 The H-series 3-1-2 The L-series 3-1-3 The PXRD measurement 3-1-4 Summary 3-2 PtRu/PPY/SBA-15 composites 3-2-1 The Si-Pt-PPY-X series 3-2-2 The Si-Pt-S-X series 3-2-3 The Si-Ru-P-S-X series 3-2-4 The Si-Ru-P-X series 3-2-5 The Si-Ru-S-X series 3-2-6 The PPY-PtRu-X series 3-2-7 The Si-PtRu-X series 3-2-8 Single metal series 3-2-9 Overall comparison 3-2-10 Cyclic Voltammetry Chapter 4. Conclusions Chapter 5. References

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