團鏈共聚物自組裝、石墨化及金屬碳合金材料之製備

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姓名

黃偉華(Wei-hua Huang) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

團鏈共聚物自組裝、石墨化及金屬碳合金材料之製備
(Electrochemically Active N-doped and N/Fe-doped Graphite with Well Defined Morphology and Dimension Fabricated from Pyrolyzed PS-P2VP Block Copolymer Nanostructures)

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摘要(中)

本研究分成兩個部分。第一個部分是以雙團鏈共聚物之自組裝奈米結構，製備具有氮摻雜之奈米碳材，第二部分則是製備含鐵/氮摻雜的奈米碳球。

第一部份探討單純高分子所製備的碳材料，首先以溶劑退火法使高分子排列成垂直柱狀、平躺柱狀以及垂直的層板結構，再利用紫外光使高分子產生交聯反應以穩定其結構，之後以高溫碳化製備出能夠複製原有高分子結構的碳材。由於組成鏈段當中含有氮原子，造成該高分子燒製的碳材會有氮原子雜化，此現象能使碳材具備將氧還原的能力。因此除了分析碳材本身的結構特性之外，也利用旋轉電極法(RDE)、循環伏安法(CV)等電化學方法，探討該材料用於氧還原電催化反應(ORR)的潛力。

第二部分是把鐵元素加入碳材當中，製備出含有氮/鐵摻雜的奈米碳球。由單純嵌段共聚物模板燒製的碳材，因為受限於高分子本身的熱裂解溫度，因此無法製備出具有較高石墨化程度的碳材料。進一步發現加入適當比例的含鐵化合物，可以大幅增加高分子在熱燒結之後的殘餘量，因此嘗試以更高的溫度對高分子進行熱燒結，最終得到石墨化程度較高的碳材。由於在極高的溫度下燒結有助於四級氮(Quaternary nitrogen)生成，而四級氮的含量與氧還原催化反應的效能呈正相關，因此加入含鐵化合物並在極高溫度下燒結的碳材除了石墨化程度增加，同時也能大幅的提高ORR的效果。進一步探討鐵的加入量對氧還原反應的影響，也比較在何種燒製條件下可以得到擁有最佳的催化特性的碳材。

摘要(英)

The research is divided as two sections. The first section is using block copolymer (BCP) self-assembled nanostructures to fabricate nitrogen-rich carbon nanomaterials, the second section is fabricating Fe/N doped carbonaceous nanomaterials.

In the first section, solvent annealing process was used to fabricate different BCP templates, such as perpendicular-oriented cylinders, lamellae, and parallel-oriented cylinders. The films were further exposed into UV-light to stabilize nanodomains; this process would increase the yield of solid carbonaceous materials during ptrolysis at elevated temperatures. As a result, the pyrolyzed graphitic nanostructures remained the original morphology of their pristine nanodomains. The pyrolysis of the nitrogen-containing block produced nitrogen-rich carbonaceous materials. The presence of nitrogen would cause an uneven distribution of electron density, giving rise to electrocatalytic activities of oxygen reduction reaction (ORR).

In the second section, Fe/N doped carbonaceous materials were fabricated. The graphitic nanostructures fabricated from thermal pyrolysis of BCP templates have low degrees of graphitization since the pyrolysis could only be achieved at a temperature close to the decomposition temperatures of the constituted blocks. An incorporation of iron-containing compounds of various fractions into the BCP template can increase the amounts of residual of solid carbonaceous materials even at much higher pyrolysis temperatures. Thus a carbonaceous material with a high degree of crystallinity can be obtained. High-temperature pyrolysis not only increased the degree of crystallinity, but also improved the amount of graphitic nitrogen. The portions of graphitic nitrogen are correlated with the performance of ORR so that the electrocatalytic activity of such Fe/N containing carbonaceous materials can be increased. Relationships between the fraction of iron-containing species and the ORR performance were found and more details were discussed in the following.

關鍵字(中)

★ 雙團鏈共聚物
★ 碳化
★ 氧氣還原反應
★ 石墨
★ 溶劑退火

關鍵字(英)

★ di-block copolymer
★ carbonization
★ oxygen reduction reaction
★ graphite
★ solvent annealing

論文目次

摘要 i

Abstract ii

目錄 iv

圖目錄 vii

表目錄 xi

第一章文獻回顧 1

1-1 高分子團鏈共聚物自組裝機制 1

1-2 塊材系統 2

1-3 溶劑退火 4

1-4 混和溶劑退火 5

1-5 形成雙團鏈共聚物微胞 7

1-6 團鏈共聚物碳化及其在電化學上的應用 8

1-7 摻入氮原子之碳材料於氧還原觸媒之研究進展 9

1-7-1 異種原子摻雜碳材之催化理論 10

1-7-2 氮原子摻雜碳材料 10

1-7-3 氮-鐵原子摻雜碳材料 13

1-8 研究動機 16

第二章實驗內容 17

2-1實驗材料 17

2-1-1 雙團鏈共聚物 17

2-1-2 溶劑 17

2-1-3 相關藥品 18

2-2 樣品製備 18

2-2-1 製備不同形貌碳材 18

2-2-2 製備孔洞結構碳材 20

2-2-3 製備Fe/N/C複合碳球 20

2-3 實驗儀器 21

2-4 儀器分析 22

2-4-1原子力顯微鏡 22

2-4-2低掠角X光散射儀 22

2-4-3 X光電子能譜 23

2-4-4 X光粉末繞射儀 24

2-4-5 拉曼光譜儀 24

2-4-6 穿透式電子顯微鏡 24

2-4-7 熱重分析儀 25

2-4-8 旋轉電極法 25

第三章結果討論 28

3-1 利用溶劑退火調控高分子微相結構 28

3-1-1利用理想氣體方程式計算溶劑退火時的氣相組成分率 28

3-1-2 製備垂直柱狀模板 29

3-1-3 製備平躺柱狀模板 31

3-1-4製備垂直層狀模板 33

3-2 高分子微相結構碳化 34

3-2-1 紫外光交聯反應對碳化的影響 34

3-2-2 燒結溫度對高分子模板的影響 35

3-2-3 碳化過程對結構有序性所造成的影響 36

3-2-4 碳化結構之鍵結組成 39

3-2-5 製備孔洞狀結構碳材 41

3-2-6 不同形貌碳材石墨化程度分析 43

3-2-7 由高分子燒結而得碳材在電化學上的應用 43

3-2-7-1 以循環還伏安法分析 44

3-2-7-2 碳材的微結構對氧還原反應的影響 45

3-3 加入鐵離子對氧還原活性的影響 48

3-3-1 鐵在碳材中的含量差異對性質造成的影響 48

3-3-1-1 在高分子中加入鐵前驅物對在碳化過程中對奈米微結構的影響 48

3-3-1-2 鐵的加入對碳膜結晶程度的影響 49

3-3-1-3 含鐵碳材之化學鍵結組成 50

3-3-1-4 以電化學方法分析含鐵量多寡對氧還原反應的差異 52

3-3-2 燒結溫度對碳材性質的影響 54

3-3-2-1 鐵加入對碳材殘餘率的影響 54

3-3-2-2 燒結溫度對含鐵碳材奈米維結構與石墨化程度之影響 55

3-3-2-3以電化學方法分析燒結溫度對氧還原反應的差異 57

3-3-2-4 比較三種不同條件對氧還原反應的影響 59

3-3-2-5 分析鐵在碳材中的結晶型態 61

3-3-2-6比較含鐵碳材在不同燒結條件的鍵結型態 62

第四章結論 64

第五章參考文獻 66

第六章附錄 75

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指導教授

孫亞賢(Ya-en Sun)

審核日期

2015-8-26

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