四面体钛基光催化氧化环己烷与环己烯的研究

发布时间：2018-08-04 10:42

【摘要】：通过浸渍法制备不同含量的硫酸氧钒改性的TS-1光催化剂以分子氧来催化氧化环己烷来合成KA油(环己醇和环己酮)。K油是工业上生产己二酸的主要原料。TS-1是由硅氧分子筛引入四面体钛形成钛氧键和四面体的硅氧键的一类催化剂。TS-1具有结构稳定、催化性能高的性质,也是一种很好的催化剂载体。TS-1的禁带宽度为3.2ev,要吸收波长小于387nm左右的紫外光才能具有光催化活性。本文通过掺杂硫酸氧钒来改变其禁带宽度,使其在可见光下具有催化活性。掺杂1%、3%、5%、7%、9%来进行研究,通过研究表明5%的催化效果最好。以分子氧为氧化剂,压力为1atm,35W的可见光为光源,反应6h,环己烷的转化率为14.5%,KA油的总选择性为94%。环己烯的氧化也引起了广大化学工作者的研究兴趣,环己烯光多相催化氧化合成过氧化环己烷、2-环己烯醇、2-环己烯酮,这几种产物均是重要的工业原料,应用广泛。采用高压反应釜不仅不能控制产物的种类,而且耗能大。本文采用光反应途径很好的解决以上问题,并且本实验不用溶剂且在常温常压下通过可见光来诱导反应。本实验采用硝酸银负载在TS-1分子筛上作为催化剂,以分子氧为氧化剂,压力为1atm,35W的可见光为光源,反应10小时,环己烯的转化率为8.6%,环己烯醇和环己烯酮的总选择性为95.5%。本实验采用了一系列的表征手段来表征催化剂,采用固体紫外光谱(UV-Vis)、傅里叶变换红外光谱(FT-IR)、氮气吸脱附、X射线荧光衍射(XRD)、X光电子能谱(XPS)、透射电镜(TEM)等。
[Abstract]:Synthesis of Ka oil (cyclohexanol and cyclohexanone) .K oil by impregnation of vanadium sulfate modified TS-1 photocatalyst using molecular oxygen to oxidize cyclohexane is the main raw material for the industrial production of adipic acid. A kind of catalyst, TS-1, which inducts tetrahedron titanium to form titanium-oxygen bond and tetrahedron silicon-oxygen bond, has a stable structure. It is also a good catalyst carrier. The band gap width of TS-1 is 3.2ev. the photocatalytic activity can be obtained only when the absorption wavelength is less than 387nm or so. In this paper, the band gap is changed by doping vanadium sulfate to make it have catalytic activity under visible light. The catalytic effect of 5% is the best. With molecular oxygen as oxidant, visible light at 1 atm ~ (35) W as light source and reaction time 6 h, the conversion of cyclohexane was 14.5kA oil and the total selectivity of the oil was 9450. The oxidation of cyclohexene has also attracted the interest of many chemists. The photo-heterogeneous oxidation of cyclohexene to cyclohexane-2-cyclohexenol 2-cyclohexenone is an important industrial raw material and widely used. The use of autoclave not only can not control the kind of products, but also consumes a lot of energy. In this paper, the light reaction approach is used to solve the above problems, and this experiment uses visible light to induce the reaction without solvent and at room temperature and atmospheric pressure. In this experiment, silver nitrate supported on TS-1 molecular sieve was used as catalyst, with molecular oxygen as oxidant, visible light source at pressure of 1 atm ~ (35) W as light source, the conversion of cyclohexene was 8.6 and the selectivity of cyclohexenol and cyclohexenone was 95.5g for 10 hours. In this experiment, a series of characterization methods were used to characterize the catalyst, such as solid ultraviolet spectroscopy (UV-Vis), Fourier transform infrared spectroscopy (FT-IR), nitrogen absorption and desorption X-ray fluorescence diffraction (XRD) X-ray fluorescence diffraction (XRD), X-ray photoelectron spectroscopy (XPS),) transmission electron microscope (TEM) and so on.
【学位授予单位】：湖南师范大学
【学位级别】：硕士
【学位授予年份】：2016
【分类号】：O621.251

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