臺灣博碩士論文加值系統

用於氧化還原反應觸媒的貴金屬，例如Pt、Pd等...，因成本過高而且稀少並限制了質子交換膜燃料電池的大規模商業化，非貴重金屬觸媒(NPMCs)的目標是取代昂貴鉑金屬觸媒，某些NPMCs不僅有高氧氣還原反應(ORR)催化活性而且便宜，以碳基材非貴金屬ORR觸媒的開發已成為燃料電池的重要課題之一。而本研究利用過度金屬鐵化合物為常見的非貴重金屬觸媒，以尿素作為氮元素的來源，經戊二醛交聯後與鐵形成錯合物。在本研究中，藉由鍛燒，使鐵、氮以及碳將在鍛燒之後形成活性位點，並藉由X-光繞射儀(XRD)、拉曼光譜儀(Raman)、功能性穿透式電子顯微鏡(cryo-TEM)、場放射型掃描電子顯微鏡(FE-SEM)、燃料電池測試設備進行觸媒性能分析。鐵/氮/碳觸媒顯現出不錯的氧氣還原反應性能和穩定性，此結果顯示鐵/氮/碳所形成的觸媒有機會發展成為質子交換膜燃料電池的陰極觸媒。

Precious metals used in redox reaction catalysts, such as Pt, Pd, etc., are too expensive and scarce and limit themass production of proton exchange membrane fuel cells. The goal of non-precious metal catalysts (NPMCs) is to replace expensive platinum metal catalysts some of NPMCs not only have high oxygen reduction reaction (ORR) catalytic activity but also are inexpensive. The development of carbon substrate non-precious metal ORR catalyst has become one of the important topics of fuel cells. In this study, the common iron compound is used as a non-precious metal catalyst, and urea is used as a source of nitrogen. After cross-linking with glutaraldehyde, it forms a network complex with iron. In this study, by calcination, iron, nitrogen and carbon will form active sites X-ray diffractometer (XRD), Raman spectrometer (Raman), functional penetration Electron microscopy (cryo-TEM), field emission scanning electron microscope (FE-SEM), and fuel cell test equipment were used for catalyst performance analysis. The iron/nitrogen/carbon catalyst exhibits good oxygen reduction reaction performance and electrochemical stability. This result indicates that the catalyst formed by iron/nitrogen/carbon owns the opportunity to develop into a cathode catalyst for a proton exchange membrane fuel cell.

摘要 I
Abstract II
誌謝 IV
目錄 V
表目錄 VIII
圖目錄 IX
第一章 緒論 1
1.1 前言 1
1.2 研究動機 2
1.3 研究架構 3
第二章 文獻回顧 4
2.1 燃料電池的發展[10] 4
2.2 燃料電池之發電原理[10] 6
2.3 燃料電池的優點 8
2.4 燃料電池種類與應用 10
2.5 質子交換膜燃料電池 12
2.5.1 PEMFC之發電原理[12-14] 13
2.5.2 質子交換膜燃料電池構造及元件 14
2.5.3 雙極版[15] 15
2.5.4 氣體擴散層 16
2.5.5 觸媒層(Catalyst Layer) 17
2.5.6 質子交換膜 19
2.5.7 膜電極組 20
2.6 非貴重金屬觸媒 21
2.6.1 氮摻雜至碳材料 21
2.7 尿素應用於觸媒[33] 23
2.8 氧氣還原反應(OXYGEN REDUCTION REACTION,ORR) 24
2.9 電極動力學 27
2.9.1 電池極化反應 27
第三章 實驗 30
3.1 實驗藥品 30
3.2 儀器設備 32
3.3 實驗步驟 35
3.3.1 配製不同比例尿素和戊二醛 35
3.3.2 氯化鐵-尿素-戊二醛聚合 35
3.3.3 觸媒合成 35
3.3.4 實驗流程反應機制 37
3.3.5 非貴重金屬之電催化氧氣還原反應(ORR)的反應機制 37
3.3.6 膜電極組(MEA)製作 38
3.3.7 MEA之單電池效率分析 40
第四章 結果與討論 42
4.1 表面型態分析 42
4.1.1 TEM分析 42
4.1.2 SEM分析 44
4.2 能量色散X-射線光譜分析(EDS、MAPPING) 46
4.3 結晶性分析(XRD) 48
4.4 官能基分析(FT-IR) 49
4.5 有序性分析(RAMAN) 49
4.6 表面性質分析(BET) 51
4.7 電化學分析(LSVS、電子轉移數) 54
4.8 單電池測試 57
第五章 結論 58
參考文獻 60

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