摘要
TS-1分子筛催化苯羟基化法制苯酚是一种绿色工艺路线。对以TS-1为催化剂苯与过氧化氢反应制苯酚的本征动力学进行了研究。考察了搅拌速度、苯浓度、过氧化氢浓度以及反应温度等因素对苯酚初始生成速率的影响,并采用幂函数方程进行实验数据拟合。结果表明,在消除内外扩散影响的条件下,反应对于苯、过氧化氢的反应级数分别为0.62和0.55,反应的活化能为101.31 kJ/mol。依据上述结果建立了反应的本征动力学方程,并对模型进行验证,结果显示模型计算得到的苯酚初始生成速率与实验值的平均相对偏差为6.81%,吻合较好。研究得到的动力学模型为TS-1催化苯羟基化-膜分离耦合制备苯酚的条件优化及过程开发提供依据。
The preparation of phenol by benzene hydroxylation over TS-1 is a green technology. The intrinsic kinetics of benzene hydroxylation to phenol with hydrogen peroxide over TS-1 was studied. The effects of agitation rate, benzene concentration, hydrogen peroxide concentration and temperature on the initial production rate of phenol were investigated, and the data were fitted by a power function equation. The results showed that when the internal and external diffusion limitations were excluded, the orders of the reaction were 0.62 with respect to benzene and 0.55 with respect to hydrogen peroxide, and the activation energy was 101.31 kJ/mol. According to the above results, the intrinsic kinetic model of benzene hydroxylation over TS-1 was established. The calculated initial production rates of phenol were in good agreement with the experimental results, and the average relative error was 6.81%. The kinetic model obtained provides the basis for the conditions optimization and process development with respect to the coupling between the benzene hydroxylation over TS-1 and the membrane separation.
出处
《化学工程》
CAS
CSCD
北大核心
2013年第11期43-47,共5页
Chemical Engineering(China)
基金
国家科技支撑计划项目(2011BAE07B05)
国家自然科学基金资助项目(20990222,21106061)
关键词
本征动力学
TS-1
苯
羟基化
苯酚
intrinsic kinetics
TS-1
benzene
hydroxylation
phenol
