雙連續相中孔二氧化鈦光催化以及電子結構之實驗與模擬研究

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姓名

呂英豪(Ying-Hao Lu) 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

雙連續相中孔二氧化鈦光催化以及電子結構之實驗與模擬研究
(Combined Experimental and Computational Study of Photocatalysis and Electronic Structure of Bicontinuous Mesoporous Titanium Dioxide)

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摘要(中)

在這項研究中，我們採用了界面活性劑和高分子聚合物作為模板並通過蒸發誘導自組裝方法製備了具有不同雙連續結構（螺旋型和原型）的中孔(mesoporous)二氧化鈦 (TiO2)。藉由界面活性劑/高分子聚合物與鈦前驅體之間的共組裝以及後續的熱處理，我們能夠獲得在分子尺度上具有銳鈦礦晶相和在介觀尺度上具有雙連續結構的二氧化鈦。利用密度泛函理論的模擬方法，我們進一步計算出不同雙連續相二氧化鈦在電子結構上的差異。透過模擬的結果以及實驗量測比表面積與帶隙，我們試圖解釋二氧化鈦於不同雙連續相結構下的光催化功效。藉由這項研究，我們希望建立催化劑的中孔結構、電子結構和催化能力三者之間的相關性。

摘要(英)

In this study, mesoporous titanium dioxide (TiO2) with different bicontinuous structures (i.e., gyroid and primitive phases) were prepared by evaporation-induced self-assembly method, where surfactants or polymers were used as templates. Via co-assembling between surfactants/polymers and the titanium precursor, followed by a heat treatment, we were able to obtain the TiO2 featured with the anatase crystalline phase in the molecular scale and bicontinuous structures in the mesoscopic scale. The photocatalytic efficacy of the mesoporous TiO2 was measured and benchmarked against the bulk Ti¬¬O2. We also determined the electronic structures for the mesoporous and bulk TiO2 through the density functional theory calculation and attempted to explain the observed differences in photocatalytic efficacy among the mesoporous and bulk TiO2 in terms of the differences in electronic structures and in experimentally determined specific surface area and band gap. Through this study, we aspire to establish correlations among mesoscopic structure, electronic structure, and catalytic capability for catalysts in general.

關鍵字(中)

★ 雙連續相
★ 二氧化鈦

關鍵字(英)

★ bicontinuous
★ titanium dioxide

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 vi
表目錄 ix
第一章緒論 1
1-1 中孔材料發展史 1
1-2 雙連續相中孔材料 4
1-3 二氧化鈦特性 6
1-4 二氧化鈦光反應及催化機制 8
1-5 雙連續相中孔二氧化鈦材料 10
1-6 研究目的及動機 12
第二章實驗方法 13
2-1 實驗藥品 13
2-2 樣品製備 14
2-2-1 陽離子雙子型界面活性劑C18-6-18合成流程 14
2-2-2 製備有機-無機複合材料流程 15
2-2-3 雙連續相銳鈦礦二氧化鈦中孔材料 18
2-3 實驗儀器 19
2-4 分析用儀器原理介紹 20
2-4-1 核磁共振光譜儀 20
2-4-2 質譜儀 23
2-4-3 X光繞射儀 24
2-4-4 小角度X光散射儀 26
2-4-5 孔洞及比表面積分析儀 29
2-4-6 紫外光/可見光分光光譜儀 32
2-5 模擬理論方法 35
2-5-1 量子力學理論演化史 35
2-5-2 軟體介紹 45
2-5-3 原子模型架構與實驗參數設定 46
第三章結果與討論 52
3-1 實驗結果分析 52
3-1-1 界面活性劑性質分析 52
3-1-2 SAXS分析 54
3-1-3 XRD分析 56
3-1-4 BET分析 57
3-1-5 UV-Vis分析 59
3-2 模擬結果分析 63
3-2-1 收斂性測試 63
3-2-2 原子結構分析 64
3-2-3 電子結構分析 65
3-3 中孔結構、能帶結構以及催化效率之相關性討論 75
第四章結論 81
文獻目錄與參考資料 82

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指導教授

陳儀帆(Yi-Fan Chen)

審核日期

2021-10-7

推文