本文關(guān)鍵詞： 環(huán)己烯 親水性 包覆 苯部分加氫 釕基催化劑　出處：《華東理工大學》2017年碩士論文　論文類型：學位論文

【摘要】：作為一種重要的有機合成中間體,環(huán)己烯具有較為活潑的C=C雙鍵,通過傳統(tǒng)水合等反應(yīng)可以制得環(huán)己醇、己二酸與己內(nèi)酰胺等工業(yè)原料。苯部分加氫制備環(huán)己烯工藝具有操作簡便、反應(yīng)路線簡單、原料來源廣泛等優(yōu)點,備受工業(yè)界青睞。然而在實際的反應(yīng)過程中,苯更傾向于發(fā)生深度加氫得到環(huán)己烷,而不是僅僅停留在中間產(chǎn)物環(huán)己烯階段。催化劑的設(shè)計在苯部分加氫過程中由此特別重要,其中催化劑表面的親水性更是發(fā)揮著關(guān)鍵作用。本研究從提高Ru基催化劑的親水性角度出發(fā),首先通過氫氣還原法制備微米尺度的Ru顆粒,并在其表面包覆親水性材料Si02和Zr02。根據(jù)苯部分加氫性能評價發(fā)現(xiàn)環(huán)己烯的收率較純Ru顆粒分別最高提高了約25.0和20.0%。在此過程中考察了親水性前驅(qū)體正硅酸乙酯(TEOS)、正丁醇鋯(TBOZ)添加量對催化劑部分加氫性能的影響以及苯部分加氫的最優(yōu)操作條件。實驗結(jié)果表明,Si02包覆Ru基催化劑的最優(yōu)反應(yīng)條件為6MPa、150℃、1000rpm、和225μL的TEOS加入量,而ZrO_2包覆Ru基催化劑最優(yōu)反應(yīng)條件為6MPa、160℃、1000rpm、和225 μL的TBOZ加入量。通過實驗證實,親水材料在Ru顆粒表面構(gòu)建的滯留水膜對于提高環(huán)己烯的選擇性具有關(guān)鍵作用,其可能作用機理在于抑制了環(huán)己烯在滯留水膜中的擴散。對同批及不同批親水性材料包覆的Ru催化劑的重復性能進行表征發(fā)現(xiàn),催化劑的重復效果良好,具有良好的工業(yè)應(yīng)用前景。
[Abstract]:As an important intermediate of organic synthesis, cyclohexene has a more active C-C bond. Cyclohexanol can be synthesized by traditional hydration reaction. Industrial raw materials such as adipic acid and caprolactam. The process of partial hydrogenation of benzene to cyclohexene has the advantages of simple operation, simple reaction route, wide source of raw materials and so on. Benzene is more inclined to produce cyclohexane by deep hydrogenation than at the intermediate product cyclohexene stage. The design of the catalyst is particularly important in the partial hydrogenation of benzene. In order to improve the hydrophilicity of Ru based catalysts, micron Ru particles were prepared by hydrogen reduction method. The hydrophilic materials Si02 and Zr02.According to the evaluation of partial hydrogenation of benzene, it was found that the yield of cyclohexene was increased by 25.0 and 20.0 than that of pure Ru, respectively. In the process, the hydrophilic precursor tetraethyl orthosilicate (TEOS) was investigated. The effect of the amount of n-butanol zirconium butanol (TBOZ) on the partial hydrogenation performance of the catalyst and the optimum operating conditions for the partial hydrogenation of benzene were investigated. The experimental results showed that the optimum reaction conditions of SiO2 coated Ru based catalyst were as follows: 6MPA 150 鈩，

本文編號：1508105