具磺酸官能基中孔洞矽材與製備奈米鈀金屬於中孔洞碳氮材在有機催化反應之應用

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陳科廷(Ke-Ting Chen) 查詢紙本館藏

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化學學系

論文名稱

具磺酸官能基中孔洞矽材與製備奈米鈀金屬於中孔洞碳氮材在有機催化反應之應用

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至系統瀏覽論文 (2026-6-30以後開放)

摘要(中)

本研究主要探討方向分為兩大部分。第一部分是利用TEOS及MPTMS為共同矽源，P123作為軟模板，在酸性環境下以雙氧水作為氧化劑，並以直接合成法的方式合成出具有磺酸官能基之中孔洞矽材K6SX及S15SX。由於K6SX及S15SX具有高比表面積以及良好的孔洞體積，並且經官能基修飾後，表面會富含磺酸官能基，藉此期望在果醣水解產出5-羥甲基糠醛(HMF)反應上會擁有良好的表現。本實驗將製成的K6SX以及S15SX應用在催化果醣水解反應上，分別探討二維結構以及三維結構、不同溫度以及不同催化劑量對催化活性之影響。經過一系列的探討，K6S20作為催化劑去進行果醣水解反應，其HMF產率可達87.42%( Ratio(Mfructose/Mcata) = 9)。在這項研究中， K6S20展示了其應用於催化果醣水解產HMF是一具高催化活性的催化劑。
而在第二部分研究中，透過三維結構之中孔洞碳材CMK-9及中孔洞碳氮材N-CMK-9作為載體，並利用化學還原劑使金屬還原速率上升，將奈米鈀金屬還原在N-CMK9及CMK-9中。CMK-9及N-CMK-9具有高比表面積以及良好的孔洞體積，此外N-CMK-9還具有缺陷的CN位點，更能使離子鈀金屬快速且平均分散在孔道之中，進而提高催化活性。本實驗將製成的Pd(X)@C9以及Pd(X)@NC9應用在催化六價鉻還原反應當中，分別探討不同載體以及不同含浸金屬量對催化活性之影響。在催化六價鉻還原反應的研究中，Pd(2)@NC9展現出很高的催化活性，其TOF值可達1.78 min-1。在這項研究中，Pd(2)@NC9展示其用於六價鉻還原催化反應中是具有高前景的催化劑。

摘要(英)

This thesis consists of two parts. In the first part, the sulfonic acid functionalized mesoporous silicas (K6SX and S15SX) have been successfully synthesized by one-pot synthesis using tetraethoxysilane (TEOS) and mercaptopropyltrimethoxysilane (MPTMS) as silicon source, P123 as a soft template and hydrogen peroxide as an oxidant in an acidic environment. According to the BET result, the surface area of K6S20 and S15S20 was confirmed about 682.6 m2/g and 452.5 m2/g. Because of the high surface area, good pore volume, and rich in sulfonic acid functional groups, K6S20 and S15S20 might have a good performance in the reaction of fructose hydrolysis to produce 5-hydroxymethylfurfural (HMF). Among all the as-prepared catalysts, K6S20 exhibited the highest HMF yield of 87.42 % at 135oC with 20 mg catalyst, 3 ml DMSO and 1 mmol fructose.
In the second part, palladium nanoparticles embedded in mesoporous N-doped carbon material (N-CMK-9), which was synthesized by nanocasting, through the double agent chemical reduction method as a catalytic catalyst. N-doped carbon material N-CMK-9 has a high surface area, good pore volume, defective CN sites and nitrogen gaps, so palladium nanoparticles could be uniformly dispersing in the materials to improve the catalytic activity. According to the TEM images, the particle size of the palladium nanoparticles was confirmed about 2-6 nm and 2-5 nm. The Pd(X)@C9 and Pd(X)@NC9 exhibited high catalytic activity for the reduction of environmentally harmful Cr(VI) to Cr (III). Among all the as-prepared catalysts, Pd(2)@NC9 exhibited the highest turnover frequency of 1.72 min-1.

關鍵字(中)

★ 奈米鈀金屬
★ 中孔洞矽材
★ 中孔洞碳氮材
★ 果醣水解反應
★ 六價鉻還原

關鍵字(英)

★ palladium nanoparticles
★ mesoporous silicas
★ mesoporous N-doped carbon material
★ fructose hydrolysis
★ reduction of Cr(VI)

論文目次

摘要 i
Abstract iii
謝誌 iv
目錄 vi
圖目錄 xi
表目錄 xvii
第一章緒論 1
第壹部分具磺酸官能基中孔洞矽材催化水解果醣 1
1-1中孔洞矽材(Ordered Mesoporous Silica, OMS) 1
1-1-1中孔洞矽材之簡介 1
1-1-2 中孔洞矽材的定義 1
1-1-3 中孔洞矽材合成方法 3
1-1-3 軟性模板-微胞結構 4
1-2 二維與三維中孔洞矽材 7
1-2-1 二維與三維中孔洞矽材之差異 7
1-2-2 二維及三維中孔洞矽材-M41S 7
1-2-3 二維中孔洞矽材-SBA-15 8
1-2-1三維中孔洞矽材-KIT-6 9
1-3 官能基化中孔洞矽材 10
1-3-1中孔洞矽材表面修飾法 10
1-3-2表面修飾含磺酸官能基之中孔洞矽材 12
1-4 果糖水解反應 16
1-4-1 羥甲基糠醛(Hydroxymethylfurfural)介紹 16
1-4-2具磺酸官能基中孔洞矽材催化果糖水解反應文獻回顧 17
第貳部分鈀金屬在中孔洞碳氮材催化鉻還原反應 21
1-5 中孔洞碳氮材 21
1-5-1 有序中孔洞碳材(Ordered Mesoporous Carbons, OMCs) 21
1-5-2 有序中孔洞碳氮材 22
1-5-3 奈米鑄模法(Nanocasting)合成機制 23
1-5-4奈米鑄模法合成有序中孔洞碳氮材之發展 24
1-6 鈀金屬催化六價鉻還原反應 31
1-6-1 六價鉻介紹 31
1-6-2 鈀金屬催化六價鉻還原機制介紹 33
1-6-3 鈀金屬催化六價鉻還原反應文獻回顧 34
1-7 研究動機與目的 37
第二章實驗部分 38
2-1 實驗藥品 38
2-2 實驗步驟 40
第壹部分具磺酸官能基中孔洞矽材催化水解果醣 40
2-2-1 合成具磺酸官能基之SBA-15(S15SX) 40
2-2-2 合成具磺酸官能基之KIT-6(K6SX) 40
2-2-4 以硫酸溶液裂解孔洞中模板 41
2-2-5 催化水解果糖實驗 41
2-2-6 催化水解果糖重複使用實驗 42
2-2-7 合成碳孔洞材料CMK9 42
2-2-8合成碳氮孔洞材料N-CMK9 43
2-2-9利用雙還原劑還原法還原奈米金屬[Pd(Y)@C9、Pd(Y)@NC9] 43
2-2-10 催化六價鉻還原反應 45
2-3 實驗設備 47
2-3-1實驗合成設備 47
2-3-2 實驗鑑定儀器 47
2-4 鑑定儀器之原理 49
2-4-1同步輻射光束線 49
2-4-2 X射線粉末繞射（PXRD） 51
2-4-3傅立葉紅外線吸收光譜儀（FTIR） 52
2-4-4固態核磁共振（Solid State NMR） 53
2-4-5氮氣吸脫附等溫曲線、表面積與孔洞特性鑑定 63
2-4-6穿透式電子顯微鏡(TEM) 68
2-4-7掃描式電子顯微鏡(SEM) 70
2-4-8元素分析儀(Elemental Analyzer；EA) 71
2-4-9光電子能譜 XPS 72
2-4-10感應偶和電漿原子發射光譜分析儀 (ICP-AES) 73
2-4-10紫外光-可見光光譜儀 (UV-Vis) 74
2-4-10高效能液相層析儀 (HPLC) 76
第三章結果與討論 77
第壹部分具磺酸官能基中孔洞矽材催化水解果醣 77
3-1材料基本性質鑑定 77
3-1-1 小角度X光繞射圖(SAXRD) 77
3-1-2 氮氣吸脫附鑑定(BET) 80
3-1-3 掃描式電子顯微鏡(SEM) 83
3-1-4 穿透式電子顯微鏡(TEM) 85
3-1-5 傅立葉紅外線吸收光譜(FT-IR) 87
3-1-6 Solid NMR 88
3-1-7元素分析(EA) 91
3-2果糖水解產HMF實驗 92
3-2-1 K6SX催化果糖水解反應 92
3-2-2 S15SX催化果糖水解反應 94
3-2-3不同材料對催化果糖水解反應之比較 96
3-2-4不同溫度對催化果糖水解反應之比較 98
3-2-5不同比例之催化劑與果糖對催化果糖水解反應之比較 100
第貳部分奈米鈀金屬催化鉻還原反應 103
3-3 材料基本性質鑑定 103
3-3-1 小角度X光繞射圖(SAXRD) 103
3-3-2 廣角度X光繞射圖(WAXRD) 106
3-3-2 等溫氮氣吸脫附鑑定(BET) 108
3-3-3穿透式電子顯微鏡(TEM) 112
3-3-4 X射線光電子能譜(XPS)及元素分析(EA) 119
3-4 奈米鈀金屬催化六價鉻還原反應實驗 124
3-4-1 Pd(X)@C9六價鉻還原 126
3-4-2 Pd(X)@NC9六價鉻還原 128
3-4-3 Pd(2)@NC9六價鉻還原之反應動力學探討 131
第四章結論 138
第五章參考資料 140

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指導教授

高憲明(Hsien-Ming Kao)

審核日期

2021-8-27

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