直接甲醇燃料電池非貴金屬陰極觸媒：鈷氮化合物之合成與應用

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姓名

陳韻宇(Yun-yu Chen) 查詢紙本館藏

畢業系所

材料科學與工程研究所

論文名稱

直接甲醇燃料電池非貴金屬陰極觸媒：鈷氮化合物之合成與應用
(Preparation and application of Co-N electrocatalyst for DMFC)

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摘要(中)

直接甲醇燃料電池(DMFC)為目前最接近商業化的燃料電池之一，由於在低溫操作，必須使用電極觸媒催化燃料及氧化劑來提升效能。目前陰極觸媒以白金為主，但白金價格一直居高不下，使得燃料電池的推動面臨一大障礙。開發可取代白金之新型非貴金屬電極觸媒為加速燃料電池商業化的首要課題之ㄧ。
本研究從碳載體種類、載體改質方法和聚吡咯摻雜量等方面針對非貴金屬陰極觸媒Co/PPy/C進行研究與開發，透過碳載體的改質技術可大幅的提升碳材表面含氧官能基，提升合成觸媒時碳材表面與觸媒前驅體的作用；也使觸媒性質由疏水性轉為親水性，增加製作MEA時塗佈觸媒的均勻性。此外，也藉由改變聚吡咯摻雜量，提高活性中心(Co-N4)數量，使觸媒活性得到提昇。

摘要(英)

Direct methanol fuel cell has all the qualities to qualify itself as the major power supply of the future and is very close to commercial realization. As a result of low temperature operation, DMFC must use catalyst to catalyze the conversion of fuels and oxidant in order to accomplish the desired efficiency. The best electrocatalyst for both conversions are platinum. The high cost and availability of platinum has become a major obstacle to the realization of DMFC. In order to solve this problem, development of non-precious electrocatalyst for DMFC is highly desirable.
In this work, we investigate the possibility of using Co/PPy/C as the cathode electrocatalysts for DMFC. Major endeavors include types of carbon support, carbon modification and the content of polypyrrole. Carbon modification was employed in order to increase the oxygen functional group on carbon surface and to promote the interaction between support surface and catalyst precursor. Furthermore, it can also control the hydropbobicity to hydrophilicity of the catalyst. This control in surface properties is essential to obtain uniformly dispersed catalyst ink in the MEA fabricating process. In addition, we also increase the the content of polypyrrole in order to increase the amount of active center(Co-N4). It can raise the activity of the catalyst in oxygen reduction reaction.

關鍵字(中)

★ 直接甲醇燃料電池
★ 鈷
★ 氧還原
★ 聚吡咯
★ 電極觸媒

關鍵字(英)

★ DMFC
★ eletrocatalyst
★ cobalt
★ polypyrrole
★ ORR

論文目次

第一章緒論 1
1.1 研究背景 1
1.2 燃料電池的歷史 2
1.3 燃料電池的基本原理與種類 4
1.4 質子交換膜燃料電池 8
1.5 電極膜組MEA 9
1.6 直接甲醇燃料電池工作原理 10
第二章文獻回顧 13
2.1 低溫燃料電池 13
2.2非貴金屬陰極觸媒發展 16
2.2.1 過渡金屬原子簇合物 17
2.2.2 中心含過渡金屬的大環化合物 17
2.2.3 Cobalt/Polypyrrole/Carbon 21
2.3 碳載體 22
第三章實驗設備與方法 25
3.1 實驗藥品與儀器設備 25
3.1.1 藥品 25
3.1.2 儀器設備 26
3.2 陰極觸媒的合成 26
3.2.1碳材表面處理 26
3.2.2針對碳纖的去雜質處理 27
3.2.3硝酸改質 27
3.2.4雙氧水改質 27
3.2.5 複合載體PPy/C合成方法 29
3.2.6 觸媒Co/PPy/C合成方法 30
3.3 性質分析 31
3.3.1 X-ray繞射分析 31
3.3.2高解析度穿透式電子顯微鏡 32
3.3.3 熱重分析儀分析 33
3.3.4 程式升溫脫附法 34
3.3.5 導電度測試 35
3.3.6 陰極觸媒活性測試 35
3.3.6.1 電極製作 36
3.3.6.2 電極特性的循環伏安法測量 37
3.3.6.3 觸媒活性計算 38
第四章結果與討論 39
4.1 研究目的 39
4.2 碳載體表面改質與測定 40
4.2.1 針對碳纖之去雜質處理 43
4.2.2 改質碳TPD與BET分析 45
4.2.3 改質碳載體導電度測定 50
4.2.4 複合載體PPy/C性質分析 51
4.2.4.1 PPy/C熱重分析 52
4.2.4.2 PPy/VGCF傅利葉紅外光譜分析 55
4.2.4.3 PPy/VGCF之SEM和TEM分析 58
4.2.4.4 PPy摻雜濃度對導電度的影響 64
4.2.5 觸媒Cobalt/Polypyrrole/Carbon性質分析 67
4.2.5.1 觸媒Co/PPy/VGCF之熱重分析 67
4.2.5.2 觸媒Co/PPy/VGCF 之XRD分析 69
4.2.5.3 觸媒Co/PPy/C之TEM分析 70
4.2.5.4 觸媒Co/PPy/C之活性分析 77
第五章結論 80
參考文獻 81

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指導教授

陳郁文(Yu-wen Chen)

審核日期

2008-7-18

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