TS-1催化苯酚羟基化制苯二酚的本征动力学研究  

Intrinsic kinetics of hydroxylation of phenol to catechol with TS-1 peroxide catalyst

作　　者：卢长娟[1] 陈日志[1] 金万勤[1] 徐南平[1] 

机构地区：[1]南京工业大学膜科学技术研究所,江苏南京210009

出　　处：《化学工程》2008年第6期38-41,共4页Chemical Engineering(China)

基　　金：国家自然科学基金资助项目(NNSFC;20636020);江苏省自然科学基金项目(BK2006722)

摘　　要：采用苯酚直接羟基化联产邻、对苯二酚被认为是目前合成苯二酚的绿色工艺路线之一,但关于以TS-1分子筛为催化剂的本征反应动力学尚在研究中。文中借助高效液相色谱技术,研究了在TS-1分子筛催化下以双氧水直接氧化苯酚为苯二酚的本征反应动力学。结果表明,当搅拌器的转速大于380 r/min时,外扩散已基本消除,反应进入动力学控制区。该反应对于苯酚和羟基化试剂双氧水的反应级数为1.2和0.53,反应活化能为76.87 kJ/mol,反应指前因子为7.58×109mol0.73/(L0.73.min)。这可为TS-1催化-膜分离耦合制备苯二酚反应过程开发和工业反应器设计提供基础数据。The preparation of catechol and hydroquinone by phenol hydroxylation is one of the most effective manufactures in the world. But there was still no report about the intrinsic kinetics of hydroxylatlon of phenol with H2O2 catalyzed by TS-1. With TS-1 as catalyst the intrinsic kinetics of the reaction of phenol with H2O2 was investigated with the help of HPLC technique. The results show that the effect of external diffusion on reaction can be ignored when the agitation rate is above 380 r/min. The order of the reaction is 1.2 with respect to phenol and 0.53 with respect to H2O2. The Arrhenius parameters were determined for overall reaction： the activation energy： Ea =76.87 kJ/mol, the pre-exponential factor：A =7.58 × 10^9 mol^0.73/（L^0.73·min）. This provides the basis for the coupling between the reaction catalyzed by TS-1 and membrane separation process and the designing of reactor.

关 键 词：本征动力学 TS-1 苯酚 羟基化 

分 类 号：O643.1[理学—物理化学]