研究生: |
林郁娟 Yu-Chuan Lin |
---|---|
論文名稱: |
高協同作用之雙摻雜氮及硫於非貴金屬觸媒應用於酸性以及鹼性氧氣還原反應之研究 Synergistic effect of N and S incorporated non-noble metal catalyst for oxygen reduction reaction in acid and alkaline media |
指導教授: |
王丞浩
Chen-Hao Wang |
口試委員: |
施劭儒
Shao-Ju Shih 梁元彰 Yuan-Chang Liang 白益豪 Yi-Hao Pai 張孫堂 Sun-Tang Chang |
學位類別: |
碩士 Master |
系所名稱: |
工程學院 - 材料科學與工程系 Department of Materials Science and Engineering |
論文出版年: | 2015 |
畢業學年度: | 103 |
語文別: | 中文 |
論文頁數: | 118 |
中文關鍵詞: | 氧氣還原反應 、燃料電池 、非貴金屬觸媒 、雙摻雜 |
外文關鍵詞: | Oxygen reduction reaction (ORR), fuel cells, non-precious metal catalyst, dual doping |
相關次數: | 點閱:430 下載:1 |
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近年來由於溫室氣體日漸上升,造成全球暖化效應,再者石油能源問題每況愈下,因此,燃料電池具有高效能、低汙染且具再生性的綠色能源變成現今最重要議題。但由於其所使用的白金觸媒昂貴,造成無法普及化之問題,因此,希望發展低價格並具高效能的非白金觸媒已成為近年來研究之趨勢。
而本研究嘗試利用含氮及含硫之前驅物以雙摻雜之方式與鐵之前驅物經由適當比例混合製備非貴金屬觸媒。發現經由700oC熱處理以及前驅物氮硫比為2:1時,其有最佳之氧氣還原能力且其電子轉移數可達3.99,已非常接近理想之電子轉移數。在結構分析上,發現此最佳化條件之觸媒,其外層有類似石墨烯層狀結構,可使觸媒導電能力提高,有助於提升氧氣還原能力。在XPS中,由氮及硫之光譜分析可得知,最佳條件之觸媒含有較多的pyridinic-N、quaternary-N及thiophene-S,此類型結構皆可大幅提升氧氣還原能力。而從XAS分析中可以了解其觸媒之鍵結形式,並從中推論其觸媒之結構。另外,將觸媒以循環伏安法(CV)方式進行30000圈穩定性測試,可得知此觸媒在反應的過程中穩定性極佳且有不錯的抗甲醇效果。
因此可證實,雙摻雜含有氮和硫於觸媒裡,藉由氮和硫之協同作用之影響,可使得氧氣還原能力得以提升。
The growing of greenhouse gases, deteriorating oils and energy issues realize people for the importance of environmental protection. Therefore, the fuel cell is significantly important due to a high efficiency, low pollution and renewable green energy. Fuel cells usually use platinum as catalyst. Unfortunately, the cost of platinum is expensive and it is not economically applied. Moreover, the resources of platinum in the world are getting scarce. Based on this view, the developing of non-noble catalysts become an attractive research topic in recent years.
This study attempts to use precursors of nitrogen and sulfur as the dual doping by mixing with iron precursors as non-noble catalyst to replace the platinum catalyst. The prepared catalyst demonstrates good oxygen reduction ability after the pyrolysis with the electron transfer number of 3.99, which is very close to the ideal electron transfer number of 4.00. From the structure analysis, the graphene-like structure is found in the outer layer, which improves the oxygen reduction activity. In XPS spectrum for nitrogen and sulfur analysis, the high amount of pyridinic-N, quaternary-N and thiophene-S structure can significantly enhance the oxygen reduction activity. From XAS analysis, we can understand the bonding of element in the catalyst and speculate catalyst structure. In addition, the catalyst has an excellent stability after 30,000 cycles of stability test. It confirms that dual-doped containing nitrogen and sulfur can enhance the oxygen reduction ability by the synergistic effect.
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