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固体酸催化剂的制备及其催化合成二芳基乙烷的研究

Preparations of Solid Acid Catalysts and Their Catalytic Synthesis of 1-phenyl-1-xylyl Ethane

【作者】 党富民

【导师】 王吉德; 宿新泰;

【作者基本信息】 新疆大学 , 无机化学, 2009, 硕士

【摘要】 二芳基乙烷(PXE)因其具有沸点高、粘度小、高溶解、凝点低、显色能力强以及耐高电压等优点,被广泛用于无碳复写纸压敏染料的溶剂及电气绝缘油等。目前,国内二芳基乙烷产品主要靠进口,市场几乎全部被国外厂商占领。因此研究新型催化合成二芳基乙烷的方法无论在理论上还是在工业上都具有重要的意义。考察了模板剂、硅铝比等制备条件对合成分子筛A1-MCM-41的影响。得出较佳合成条件为:以硅酸钠为硅源,硫酸铝为铝源,以CTAB为模板剂,采用水热法合成了负载型固体酸A1-MCM-41介孔分子筛。并通过X射线衍射(XRD)、热重差热分析(TG-DTA)、扫描电镜(SEM)、透射电镜(TEM)和红外(IR)等对其进行了表征,从而检测了催化剂的活性物质组成、结构。考察了磷钨酸负载型固体酸催化剂的制备条件,其较佳制备条件为:以HM沸石为载体,采用超声浸渍法制备了的磷钨酸负载型固体酸PW-HM催化剂,并通过XRD、IR、SEM和TEM等方法对其进行了表征。主要研究了包括Al-MCM-41分子筛和丝光沸石负载磷钨酸型固体酸两类催化剂。同时对该催化剂催化合成二芳基乙烷的合成工艺进行了研究。得出较佳合成条件为:原料苯乙烯与二甲苯质量之比为1∶7 .5,反应温度为140℃,催化剂用量为1 %(总投料质量百分比),反应时间为3 h,产率可达87.1 %,比传统催化剂浓硫酸提高了17 %,研究结果表明,该催化剂是替代传统液体酸催化剂合成二芳基乙烷的理想固体酸催化剂,可以消除以往用液体酸作为催化剂时对设备的腐蚀,避免产生大量的废酸、废水等。为实现以固体酸为催化剂催化合成二芳基乙烷提供了理论依据。

【Abstract】 Diphenylethane (PXE) is a colorless synthetic liquid with many excellent properties, such as high-boiling point, small viscosity, low-pour point, strong color ability and high voltage-resistance,which are suitable for various industrial applications, e.g., a solvent for pressure-sensitive record materials, electric-insulating oil etc. At present, The PXE products depend mainly on abroad. So it is significant to study new catalytic synthesis methods of PXE both theoretically and industrially.The effects of preparation conditions such as the templates, Si-Al ratio on the synthesis of molecular sieve A1-MCM-41 were discussed. The results showed that the optimal conditions were: Na2SiO3 as silica source, Al2(SO4)3 as aluminum source, and cetyltrimethylammonium bromide (CTAB) as template agent under hydrothermal condition. The composition and configuration of A1-MCM-41 molecular sieve are determined by characterization of X-ray diffraction (XRD), thermogravimetry differential thermal analysis (TG-DTA), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and infrared spectroscopy (IR).The proper conditions of preparating supported catalyst PW/HM have been obtained: it was prepared by ultrasonic treatment during the impregnation step, with HM zeolite as a carrier. Structural and physical properties of the catalysts were characterized by XRD、IR、SEM and TEM.Two kinds of catalysts Al-MCM-41 mesoporous sieves catalysts and H3PW12O40 supported mordenite(HM)catalysts have been prepared in this thesis. The synthesis of diphenylethane with these catalysts and their catalytic performance were investigated. The optimal conditions were: the mass percent of catalyst was 1 % of feed stock; the weight ratio of xylene to styrene was 7.5: 1; the reaction temperature was 140°C and the time was 3 h. The yield of diphenylethane under such conditions was about 87.1 %, which was 17 % higher than that catalyzed by sulfuric acid. The results showed that Al-MCM-41 and PW-HM might be promising solid acid catalysts instead of liquid acid for synthesis of diphenylethylane. The solid acid can be used to eliminate the corrosion of equipment, and avoid discharge of waste acid and waste water. This work provides a theoretical basis on systhesizing PXE with solid acid as catalyst.

【关键词】 固体酸Al-MCM-41丝光沸石二芳基乙烷催化
【Key words】 solid acidAl-MCM-41mordenitediphenylethanecatalysis
  • 【网络出版投稿人】 新疆大学
  • 【网络出版年期】2010年 01期
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