介孔Fe-MCM-41纳米粒子的合成及其在催化反应中的应用-无机化学专业论文.docxVIP

哈尔滨工业大学理学硕士学位论文 哈尔滨工业大学理学硕士学位论文 -II- -II- Abstract Pure silica MCM-41 with weak acidity has no catalytic activity in selective oxidation reaction. Iron-substituted MCM-41 has better catalytic activities via incorporation of iron in the mesoporous framework. Furthermore, particle size plays an important role in the catalytic properties, that is, mesoporous nanoparticles display improved catalytic performance in some catalytic reactions compared with corresponding large particles. In this paper, ordered Fe-MCM-41 nanoparticles with various iron contents were successfully prepared via room-temperature method, in which NaOH and CTAB were used as alkaline source and surfactant, respectively. The samples were characterized by SEM, TEM, XRD, N2 adsorption-desorption isotherms measurement, FT-IR and UV-vis spectroscopy. Besides, effects of the content of NaOH, CTAB and iron source on the mesoporous structures were investigated. Additionally, ordered Fe-MCM-41 nanoparticles were obtained by the post-synthesis method. The samples prepared by the two synthetic methods were used to be catalysts in phenol hydroxylation with H2O2 as oxidant. It was found that Fe-MCM-41 nanoparticles indicated higher initial reaction rate and effective utilization of hydrogen peroxide, achieving the given phenol conversion at a shorter reaction time. This is mainly because mesoporous nanoparticles can facilitate the diffusion of reactant molecules in the shorter mesoporous channels. In addition, Fe-MCM-41 nanoparticles can be catalyst for Friedel-Crafts reaction with benzyl chloride and benzene, in which benzyl chloride conversion could be up to 100% in a short time. Keywords: Fe-MCM-41 nanoparticles, room-temperature method, post-synthesis method, phenol hydroxylation, Friedel-Crafts -III- -III- 目 录 摘 要 I AbstractII 第 1 章 绪 论 1 1.1 课题背景及研究的目的和意义 1 1.2 介孔材料的历程 2 1.3 介孔材料的机理和方法 4 1.3.1 合成机理 4 1.3.2 合成方法 5 1.4 介孔材料的改性 6 1.4.1 形貌控制 6 1.4.2 孔径调节 7 1.4.3 水热稳定性提高 8 1.5 杂原子 MCM-