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研究生: 劉彥辰
Liu, Yan-Chen
論文名稱: 複合氣凝膠之製備與其觸媒性質之探討
An Investigation of the Preparation and Catalytic Properties of Composite Aerogels
指導教授: 吳志勇
Wu, Chih-Yung
學位類別: 碩士
Master
系所名稱: 工學院 - 太空系統工程研究所
Institute of Space Systems Engineering
論文出版年: 2026
畢業學年度: 114
語文別: 中文
論文頁數: 89
中文關鍵詞: 二氧化矽氣凝膠複合金屬氧化物觸媒鑭鈰鈷錳氧過氧化氫催化分解
外文關鍵詞: silica aerogel, composite metal oxide catalyst, La-Ce-Co-Mn-O, catalytic decomposition of hydrogen peroxide
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  • 過氧化氫因分解產物主要為水與氧氣,且相較於聯胺類推進劑具有毒性較低及操作安全性較高等優點,被視為具發展潛力之綠色推進劑。然而,其分解反應高度依賴觸媒材料之組成、表面活性與孔洞結構,因此開發兼具良好催化活性與多孔特性之非貴金屬觸媒具有重要意義。
    本研究以二氧化矽氣凝膠作為多孔載體,導入La、Ce、Co及Mn等金屬元素,製備不同組成之金屬氧化物/SiO2複合觸媒。樣品經溶膠-凝膠、真空乾燥及煅燒程序後,利用場發射掃描式電子顯微鏡、能量散射光譜、X射線繞射及氮氣吸附-脫附分析,探討其表面形貌、元素分布、晶相組成與孔洞特性,並以95 wt.%高濃度過氧化氫進行排水集氣測試,以評估各樣品之初期表觀催化活性。
    分析結果顯示,金屬元素可分散於SiO2載體中,不同金屬組成會影響材料之顆粒形貌、結晶特性及孔洞結構。金屬氧化物導入後,樣品比表面積與孔體積雖有所降低,但仍保有以中孔為主之多孔結構,有助於反應物傳輸及活性位點接觸。催化測試結果顯示,含Co之樣品整體具有較佳之過氧化氫分解能力,其中La-Ce-Co-Mn-O/SiO₂複合觸媒之反應時間最短,呈現最佳初期表觀催化活性。
    綜合而言,觸媒性能並非僅由比表面積決定,亦受到金屬組成、晶相結構、元素分散程度與多價態金屬氧化還原能力等因素共同影響。La-Ce-Co-Mn-O複合氧化物與SiO2多孔載體之結合,可兼顧活性相分散與催化反應能力,具有應用於高濃度過氧化氫分解觸媒及綠色太空推進系統之發展潛力。

    Hydrogen peroxide (H2O2) is considered a promising green propellant because its decomposition products are mainly water and oxygen, while its toxicity is lower than that of conventional hydrazine-based propellants. However, the decomposition performance of H2O2 strongly depends on catalyst composition, surface activity, and pore structure. In this study, porous SiO2 was used as a support and combined with Mn, Co, La, and Ce to prepare Mn-O/SiO2, La-Mn-O/SiO2, Co-O/SiO2, La-Co-O/SiO2, and La-Ce-Co-Mn-O/SiO2 composite catalysts. The samples were prepared through sol-gel processing, vacuum drying, and calcination, and were characterized by FE-SEM, EDS, XRD, and nitrogen adsorption-desorption analysis. Catalytic performance was evaluated using 95 wt.% H2O2 with a water-displacement gas collection method. The results showed that metal loading reduced the specific surface area and pore volume, but the composite samples still retained mainly mesoporous structures. Co-containing samples exhibited better catalytic performance than Mn-based samples. La-Ce-Co-Mn-O/SiO2 showed the shortest reaction time of 12.93 ± 0.91 s and the highest initial apparent catalytic activity.

    摘要 i Extended Abstract ii 誌謝 vi 目錄 ix 圖目錄 xi 表目錄 xiii 縮寫表 xiv 第1章 序論 1 §1-1 前言 1 §1-2 研究動機與目的 3 第2章 文獻回顧 6 §2-1 氣凝膠材料概述 6 2.1.1 氣凝膠之定義與基本特性 7 2.1.2 氣凝膠之孔洞結構與比表面積 7 2.1.3 氣凝膠於觸媒載體之應用潛力 8 §2-2 二氧化矽氣凝膠之製備與性質 8 2.2.1 二氧化矽氣凝膠之材料特性 8 2.2.2 溶膠-凝膠法製備原理 9 2.2.3 水解與縮合反應機制 10 2.2.4 乾燥方式對孔洞結構之影響 11 2.2.5 二氧化矽氣凝膠作為觸媒載體之優勢與限制 11 §2-3 鈣鈦礦型氧化物觸媒 11 2.3.1 鈣鈦礦型氧化物之結構特性 11 2.3.2 A位與B位元素取代對觸媒性質之影響 12 2.3.3 La-Ce-Co-Mn-O鈣鈦礦型觸媒之研究 12 §2-4 過氧化氫觸媒 14 第3章 研究方法與實驗設備 15 §3-1 研究方法 15 3.1.1 SiO2氣凝膠製備程序 15 3.1.2 金屬氧化物/SiO2氣凝膠複合觸媒製備程序 18 §3-2 藥品與材料21 §3-3 儀器設備22 3.3.1 場發射掃描式電子顯微鏡分析(FE-SEM) 24 3.3.2 X射線繞射分析(XRD) 27 3.3.3 比表面積與孔徑分布分析(BET)28 3.3.4 X 射線光電子能譜儀(XPS) 31 §3-4 過氧化氫催化性能測試 32 第4章 結果與討論 33 §4-1 觸媒材料性質分析 33 4.1.1 FE-SEM表面形貌分析 33 4.1.2 Mapping表面元素面掃描分析 43 4.1.3 XRD結構分析 50 4.1.4 BET比表面積分析 55 4.1.5 XPS表面化學態分析 57 §4-2 觸媒催化性質分析 63 第5章 結論與未來展望 66 §5-1 結論 66 §5-2 未來展望 67 參考文獻 69

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