具水熱穩定乙烷基官能基與磺酸官能基之中孔洞材料 SBA-1 的合成與鑑定

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鄭光良(Guang-Liang Jheng) 查詢紙本館藏

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具水熱穩定乙烷基官能基與磺酸官能基之中孔洞材料 SBA-1 的合成與鑑定
(Synthesis and Characterization of Hydrothermally Mesoporous Stable Silicas SBA-1 Functionalized with Ethylane-bridge and Sulfonic Acid Groups)

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摘要(中)

本篇研究主要為合成具高水熱穩定性之中孔洞分子篩，使用 BTEE (1,2-Bis(triethoxysilyl)ethane)及TEOS (Tetraethyl orthosilicate) 為共同矽源，以 C16TEABr (Cetyltriethylammonium bromide) 作為模板試劑，在酸性條件下直接合成含有乙烷有機官能基的 cubic (Pm3n) 中孔洞材料。經由粉末 X-ray 繞射、等溫氮氣吸脫附 (BET)、29Si 及 13C MAS-NMR、掃描電子顯微鏡 (SEM)、熱重分析儀 (TGA) 做鑑定。將模板移除後的樣品在沸水下迴流，藉此與純的 SBA-1 比較其水熱穩定性。然而，結果顯現出在混合矽源下合成其結構在經五天水煮後還保持部分的結構特性，相較於水煮一天結構就崩塌的純 SBA-1，此共同矽源明顯改善其水熱穩定性。
在另一部份則是使用TEOS與 MPTMS ((3-Mercaptopropyl)- trimethoxy silane) 為共同矽源，以 C16TEABr作為模板試劑，在酸性條件下以雙氧水當作氧化劑，利用直接合成將硫基官能基轉變成含有磺酸基有機官能基的中孔洞材料。然而，適量的雙氧水可促進其磺酸基的生成。藉由粉末 X-ray 繞射、等溫氮氣吸脫附 (BET)、29Si 及 13C MAS-NMR 鑑定之。
然而，重金屬的檢測及定量在區域的環境監控、污水管理，甚至生物演變在近年來雖然利用很多不同儀器的技術進行檢測，但在此將利用硫基對不同金屬的吸附性，以固態核磁共振儀鑑定之。除此之外，也發現也許可在不需要雙氧水的形況下，利用銅金屬將硫基轉換為磺酸基。

摘要(英)

Hydrothermally stable periodic mesoporous organosilicas with cubic Pm3n frame structures were synthesized by using tetraethoxysilane (TEOS) and 1,2-bis(triethoxysilyl)ethane (BTEE) as silica source and cetyltriethylammonium bromide (CTEABr) as surfactant under acidic conditions.The synthesized materials were characterized by PXRD, SEM, N2 adsorption-desorption, 29Si MAS NMR, 13C CP MAS NMR and TG-DTA techniques. Hydrothermal stability of the synthesized material was evaluated by refluxing the sample under boiling water for various time periods and the results were compared with pure mesoporous silica material (Si-SBA-1). The results showed that the hybrid material is stable up to 5 days in boiling water with a slight decrease in structural properties, whereas Si-SBA-1 structure was collapsed after refluxing for one day. The improved hydrothermal stability of hybrid material is related to more hydrophobic environment induced inside the pore channels due to the presence of integrating ethane groups in the walls of the channels.
On the synthesis of organosulfonic acid-functionalized mesoporous in a one-step approach of co-condensing inorganic–organic reagents in the presence of cetyltriethylammonium bromide (CTEABr) surfactant with in situ oxidation of the thiol groups to the sulfonic acid groups.It is a one-step condensation of tetramethoxysilane (TEOS) and 3-mercaptopropyltrimethoxysilane (MPTMS) in highly acidic medium. During the condensation process, the in situ oxidation of thiol (-SH) group to sulfonic acid (-SO3H) group was facilitated by hydrogen peroxide (30 wt % H2O2). Adsorption and structural properties of the aforementioned PMOs have been studied by nitrogen adsorption and X-ray diffraction, whereas their framework chemistry was quantitatively analyzed by solid-state 13C and 29Si MAS NMR.
The detection and quantification of heavy metal ions are important in plethora of areas such as environmental monitoring, waste water management, developmental biology, and clinical toxicology. A number of techniques have been developed over the years for heavy metal ion analysis. Now, we used solid-state 13C CPMAS (cross polarization magic angle spinning) NMR spectroscopy as a characterization tools to obtain spectroscopic evidence for the heavy metal adsorption. By the way, the conversion of thiol-functionalized SBA-1 to disulfide-functionalized SBA-1 using Cu2+ without hydrogen peroxide was achieved.

關鍵字(中)

★ 水熱穩定
★ 乙烷
★ 硫基

關鍵字(英)

★ Hydrothermally
★ Sulfonic Acid
★ Ethylane-bridge

論文目次

中文摘要................................................................................................... I
英文摘要.................................................................................................. II
目錄......................................................................................................... IV
圖目錄................................................................................................... VIII
表目錄.................................................................................................... XII
第一章序論............................................................................................... 1
1-1 中孔洞分子篩材料歷史.............................................................. 1
1-2 觸媒簡介...................................................................................... 6
1-3 界面活性劑性質簡介.................................................................. 7
1-4 微胞的形成與種類...................................................................... 8
1-5 SBA-1 簡介................................................................................. 10
1-6 SBA-1 的形成機制..................................................................... 12
1-7 官能基化中孔洞分子篩簡介.................................................... 13
1-8 文獻回顧.................................................................................... 15
1-9 表面修飾中孔洞分子篩之應用................................................ 19
1-10 研究動機與目的...................................................................... 22
第二章實驗部分..................................................................................... 23
2-1 藥品............................................................................................ 23
2-2 實驗步驟.................................................................................... 25
2-2.1 合成界面活性劑 CTEABr............................................... 25
2-2.2 合成含乙烷基官能基的SBA-1(BTEE-SBA-1) ............. 25
2-2.3 合成含乙烷基官能基的SBA-1(BTEE-SBA-1) ............. 26
2-2.4 以溶劑萃取法移除SBA-1 孔洞中的模板...................... 29
2-2.5 中孔洞分子材料 SH-SBA-1 吸附金屬離子實驗…..... 30
2-3 實驗設備.................................................................................... 30
2-3.1 實驗合成設備................................................................... 30
2-3.2 實驗鑑定儀器................................................................... 30
2-4 鑑定儀器之原理........................................................................ 31
2-4.1 X 光繞射 (Powdr X-Ray Diffractometer；XRD)............ 31
2-4.2 氮氣吸脫附等溫曲線、表面積與孔洞特性鑑定......... 34
2-4.3 傅立葉紅外線吸收光譜 (FTIR)...................................... 38
2-4.4 熱重分析儀 (Thermo Gravimetric Analyzer；TGA)...... 40
2-4.5 固態核磁共振 (Solid State NMR)................................... 40
2-4.5-1 去氫偶合 (proton decoupling)................... .............. 41
2-4.5-2 魔角旋轉 (Magic Angle Spinning)............... ........... 41
2-4.5-3 交叉極化 (Cross-Polarization, CP).............. ............ 42
2-4.5-4 異核間作用力 (Heteronuclear Correlation, Hetcor)..43
2-4.6 低真空掃描式電子顯微鏡 (LV-SEM)………………….. 45
2-4.7 元素分析儀 (Elemental Analyzer；EA)........................... 46
2-4.8 感應耦合電漿原子發射光譜分析儀 (ICP-AES)............ 47
第三章結果與討論................................................................................ 48
3-1 不同比例下混合矽源合成的 BTEE-SBA-1 ........................... 48
3-1-1.1 XRD 結果.................................................................... 48
3-1-1.2 氮氣等溫吸脫附的結果.............................................. 50
3-1-1.3 13C CP/MAS NMR 結果............................................. 54
3-1-1.4 29Si MAS NMR 結果.................................................. 56
3-1-1.5 HETCOR - 2D MAS NMR 結果................................ 60
3-1-1.6 FT-IR 結果........................................ ......... ................ 64
3-1-1.7 TGA 結果.................................................................... 66
3-1-1.8 SEM 結果 .................................................................. 71
3-1-1.9 水氣等溫吸附的結果.................................................. 73
3-1-2 不同水煮時間下探討中孔洞材料 BTEE-SBA-1 ................ 76
3-1-2.1 XRD 結果 .................................................................. 76
3-1-2.2 氮氣等溫吸脫附的結果.............................................. 79
3-2 不等量雙氧水氧化SH-SBA-1 為SO3H-SBA-1 ..................... 89
3-2-1.1 XRD 結果 .................................................................. 89
3-2-1.2 13C CP/MAS NMR 結果 ........................................... 93
3-2-2 氧化不同比例SH-SBA-1 為SO3H-SBA-1 .......................... 97
3-2-2.1 XRD 結果.................................................................... 97
3-2-2.2 氮氣等溫吸脫附的結果.............................................. 99
3-2-2.3 13C CP/MAS NMR 結果.............................................102
3-2-2.4 29Si MAS NMR 結果................................................. 104
3-2-2.5 HETCOR - 2D MAS NMR 結果.............................. 107
3-2-2.6 TGA 結果.................................................................. 110
3-2-2.7 酸催化反應結果...................................................... 112
3-3 金屬離子的吸附 ..................................................................... 114
3-3-1 XRD 結果......................................................................114
3-3-2 13C CP/MAS NMR 結果 .............................................118
3-3-3 ICP-AES 結果.............................................................. 122
3-3-4 銅離子催化結果......................................................... 125
3-3-4.1 XRD 結果 ............................................................ 125
3-3-4.2 13C CP/MAS NMR 結果....................................... 127
第四章結論............................................................................................ 129
參考文獻................................................................................................ 130

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指導教授

高憲明(Hsien-Ming Kao)

審核日期

2008-7-21

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