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目 SBA15 介孔分子篩的改性及 其催化性能研究 學生姓名 學 號 院(系) 專 業(yè) 化學工程與工藝 指導(dǎo)教師 時 間 20xx年 6月 8日 第 I 頁 摘要 介孔分子篩 SBA15 具有較高比表面積、規(guī)則孔道結(jié)構(gòu)及孔徑易于控制、熱穩(wěn)定性和水熱穩(wěn)定性較好、表面易官能化等特點,在催化化學和吸附分離等領(lǐng)域有廣闊的應(yīng)用前景。本研究旨在采用浸漬法對 SBA15 介孔分子篩進行功能化修飾,以便引入酸性中心。結(jié)果表明: 負載改性后的 SBA15 仍保持規(guī)整的孔道排列和六方相介孔結(jié)構(gòu) 并具有一定強度的酸性 。 關(guān)鍵詞 : REAl/SBA15;稀土改性;酯化;烷基化 第 II 頁 Abstract The mesoporous molecular sieve SBA15 has attracted considerable attention in the fields of catalytic chemistry and adsorptionseparation, due to high surface area, uniform pore size and tunable pore structure, high thermal and hydrothermal stability easily functionalized surface. The point of research on mesoporous materials currently focuses on the exploitation of their application in catalysis. Via using appropriate precursors and preparation methods, the functional modification of mesoporous materials has played considerable roles in improving the performance of catalytic properties. Because of the weak acidicity, SBA15 can’t be used as acidic catalyst unless a heteroatom was introduced into its skeleton because some acid centers were obtained. The purpose in this study is to functional modification of SBA15 mesoporous molecular sieves by the impregnation method for the incorporation of acid sites. The mesoporous molecular sieves SBA15 were synthesized by hydrothermal synthesis method and modified by incorporating Al atoms and RE (La, Ce). Moreover, the modified REAl/SBA15 catalytic activity was investigated in the esterification reaction of acetic acid and ethanol, alk ylation reaction of tertbutyl alcohol and phenol. The REAl/SBA15 was characterized by XRD, N2 adsorptiondesorption, TEM, 27Al NMR, NH3TPD and PyIR, which demonstrated that the REAl/SBA15 maintained the primary hexagonally ordered mesoporous structure and a certain intensity of acidity. The mesoporous molecular sieve catalyst REAl/SBA15 was used for esterification reaction, and the effects of doping amount of La and Ce, reaction temperature, reaction time, species of the catalysts were investigated, respectively. It showed that the catalytic performance of REAl/SBA15 is poor in esterification reaction , due to the moderate acid center. However LaAl/SBA15 exhibited high catalytic activity in the alkylation reaction of tertbutyl alcohol and phenol, which achieved the highest conversion of phenol was % and the sum of selective of three main target product(4TBP, 2,4DTBP, 2TBP) was % under the following conditions: molar ratio of tertbutyl alcohol and phenol 4:1, catalyst amount , reaction temperature 190℃ and reaction time 2 h. 第 III 頁 Keywords: REAl/SBA15, Rare earth, Esterification , Alkylation 第 i 頁 目錄 摘要 ............................................................................................................................... I Abstract ........................................................................................................................II 第 1 章緒論 .................................................................................................................. 1 介孔材料概述 ............................................................................................... 1 介孔材料的分類 ................................................................................ 2 介孔分子篩的制備及其機理 ............................................................ 3 介孔分子篩 SBA15 概述 ............................................................................ 5 介孔分子篩 SBA15 的合成 ............................................................. 5 介孔分子篩 SBA15 修飾與改性 ..................................................... 6 介孔分子篩 SBA15 在催化領(lǐng)域的應(yīng)用 ..................................... 10 本論文 研究思路 及課題內(nèi)容 ................................................................... 12 本研究的催化反應(yīng)(乙酸與乙醇的酯化和叔丁醇與苯酚的烷基化) . 12 第 2 章實驗材料與實驗方法 .................................................................................... 14 主要實驗試劑及實驗儀器 ....................................................................... 14 主要實驗試 劑 ................................................................................ 14 主要實驗儀器設(shè)備 .......................................................................... 15 樣品的表征分析方法 ............................................................................... 15 小角 X 射線衍射分析 ................................................................... 15 N2 吸附 脫附分析 .......................................................................... 15 透射電子顯 微鏡表征 .................................................................... 16 27Al 魔角旋轉(zhuǎn)固體核磁共振譜表征分析 ................................... 16 吡啶吸附的紅外光譜分析 ............................................................ 16 氨氣程序升 溫脫附法分析 ............................................................... 16 催化活性分析 ........................................................................................... 17 乙酸與乙酯酯化反應(yīng)活性分析 .................................................... 17 苯酚叔丁醇烷基化反應(yīng)活性分析 ................................................... 17 第 3 章 REAl/SBA15 的合成及其表征分析 ...................................................... 19 引言 ........................................................................................................... 19 SBA15 與 REAl/SBA15 的合成 .......................................................... 19 第 ii 頁 水熱法合成 SBA15.....................................