簡淑華臺灣大學：化學研究所張仁偉Chang, Ren-WeiRen-WeiChang2007-11-262018-07-102007-11-262018-07-102006http://ntur.lib.ntu.edu.tw//handle/246246/51746Titanium-containing SBA-15 (Ti-SBA-15) was synthesized via a modified hydrothermal method, prepared as following: an amount of triblock copolymer P123 (EO20PO70EO20) was dissolved in 1 M HCl solution, followed by the dropwise addition of a mixture of tetraethylorthosilicate (silicon source, TEOS) and tetraethylorthotitanate (titanium source, TBOT) with the desired ratio of Ti and Si (in mole). After stirring 24 h, adding some amount of 2 M NaOH solution to adjust the desired pH of the synthesis system, and then hydrothermal treatment at 80 ℃ for 24 h. The final solid was collected by filtration, washed with water, and dried at room temperature, and then calcinated at 550 ℃ for 6 h. The structure characterization of Ti-SBA-15 and its photocatalytic properties was investigated. The element analysis results indicated that the amounts of titanium in pH-adjusted Ti-SBA-15 are higher than that of Ti-SBA-15 as much as one order of magnitude. HRTEM images of all Ti-SBA-15 show well-ordered hexagonal arrays of mesopore with one-dimensional channels, and TiO2 aggregated layer at outside surface of pH-adjusted Ti-SBA-15 was observed. With increasing the pH value of the synthesis system, some TiO2 aggregated seriously to form nanoparticles anchored on the surface of Ti-SBA-15. N2 adsorption isotherm (77 K) shows the adsorption type of all Ti-SBA-15 are type Ⅳ with H1 hysteresis loop, which is typical for mesoporous materials with 2-D-hexagonal structure. From UV-Visible spectrum, Ti/Si = 0.05 shows the absorption band at 200-250 nm, indicated that titanium at framework site. When Ti/Si ratio increased, another adsorption band at about 300 nm emerges, indicated titanium distributed at extraframework site. X-ray adsorption spectrum evidenced that titanium at four coordination state in Ti-SBA-15, and titanium mainly at six coordination state in pH-adjusted Ti-SBA-15. From pyridine adsorption IR spectrum, all Ti-SBA-15 show Lewis acid properties. Nitric oxide photocatalytic analysized by in-situ Electron Paramagnetic Resonance (in-situ EPR) indicated that Ti-SBA-15 adjusted pH=1 has the best photocatalysis for NO degradation with high nitrogen selectivity in products. Simultaneously, the photodegradation test of salicylic acid also shows that Ti-SBA-15 adjusted pH=1 exhibited the best performance. The high photocatalytic activity of Ti-SBA-15 adjusted pH=1 is contributed to TiO2 layer distributed uniformly at the outside surface of molecular sieves.目錄 第一章 緒論 1-1 中孔洞氧化矽分子篩簡介……………………..……….…1 1-2 二氧化鈦光觸媒…………………………………..……….4 1-3 研究動機…………………………………………...………8 第二章 實驗 2-1 化學藥品………………………………………………...9 2-2 合成步驟…………………………………………………10 2-3 特性分析 2-3.1 觸媒之結構鑑定………………………………….12 2-3.2 觸媒之形態鑑定………………………………….13 2-3.3 觸媒之表面積、孔徑與孔體積鑑定…………….13 2-3.4 觸媒之組成分析…………………………….……14 2-3.5 觸媒之表面組成分析………………………….…14 2-3.6 觸媒之酸性鑑定…………………………….……15 2-4 光催化反應測試 2-4.1原位電子順磁共振光譜 ( in-situ EPR )分析系統 – ㄧ氧化氮吸附與光催化反應……………………….......18 2-4.2 柳酸光催化分解反應……………………….……22 第三章 結果與討論 3-1. 分子篩之合成與特性分析 3-1.1 初始Ti/Si = 0.05製得之含鈦分子篩……………...23 3-1.2 初始Ti/Si = 0.10製得之含鈦分子篩………….....47 3-1.3 初始Ti/Si = 0.20製得之含鈦分子篩…………….…60 3-2 光催化反應 3-2.1 in-situ EPR NO的吸附及光催化分解活性…….71 3-2.2 柳酸光催化分解………………………….......76 3-3 綜合討論……………………………................81 第四章 結論………………………………………………..…84 參考文獻………………………………………………………..85 附錄1 AAS鈦、矽、鈉三元素之檢量線……………………..884648851 bytesapplication/pdfen-US含鈦SBA-15一氧化氮光分解柳酸光分解Titanium-containing SBA-15NO photodecompositionphotodegradation of salicylic acidthesishttp://ntur.lib.ntu.edu.tw/bitstream/246246/51746/1/ntu-95-R93223069-1.pdf