催化学报 ›› 2007, Vol. 28 ›› Issue (3): 222-228.

• 研究论文 • 上一篇    下一篇

Fe-MSU-1介孔分子筛的合成及其催化苯酚羟基化性能

刘红,王志刚,李浩   

  1. 上海大学化学工程与工艺系, 上海 201800
  • 收稿日期:2007-03-25 出版日期:2007-03-25 发布日期:2007-03-25

Synthesis of Fe-MSU-1 and Its Catalytic Properties for Hydroxylation of Phenol

LIU Hong*, WANG Zhigang, LI Hao   

  1. Department of Chemical Engineering, Shanghai University, Shanghai 201800, China
  • Received:2007-03-25 Online:2007-03-25 Published:2007-03-25

摘要: 以月桂醇聚氧乙烯醚为模板剂,在中性条件下成功合成了Fe-MSU-1介孔分子筛. 采用X射线衍射、傅里叶变换红外光谱、紫外-可见吸收光谱、电子自旋共振谱、透射电镜、低温N2吸附和电感耦合等离子体原子发射光谱对样品进行了表征. 考察了Fe-MSU-1分子筛在苯酚羟基化反应中的催化性能以及工艺条件对苯酚羟基化反应的影响. 结果表明, Fe3+离子进入了分子筛骨架, Fe-MSU-1分子筛具有均一的蠕虫状介孔结构,平均孔径约为2.9 nm. 在焙烧后的Fe-MSU-1样品中, Fe3+主要以四配位的形式存在,无骨架外Fe2O3物种形成. 以水为溶剂,在苯酚/H2O2摩尔比为3, 反应温度353 K, 反应时间7 h的条件下,苯酚和H2O2的转化率以及苯二酚的选择性分别达到20.4%, 96.9%和99.6%.

关键词: 铁, MSU-1介孔分子筛, 苯酚, 羟基化

Abstract: Iron-incorporated mesoporous silica material Fe-MSU-1 was successfully synthesized using lauryl alcohol-polyoxyethylene (23) ether as the templating agent under the neutral pH condition. The sample was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, ultraviolet-visible absorption spectroscopy, electron spin resonance, transmission electron microscopy, N2 adsorption, and inductively coupled plasma-atomic emission spectroscopy. Its catalytic performance for hydroxylation of phenol was studied. The effects of catalyst concentration, solvents, phenol/H2O2 molar ratio, reaction temperature, and reaction time on the hydroxylation of phenol over the Fe-MSU-1 catalyst were examined. The results showed that Fe3+ ions were successfully incorporated into the framework of MSU-1, and the Fe-MSU-1 material had a uniform worm-like mesoporous structure with about 2.9 nm pore diameter. After calcination, Fe3+ ions were mainly present in tetrahedral coordination, and no extraframework Fe2O3 was formed. Under the conditions of water solvent, n(phenol)/n(H2O2)=3, reaction temperature 353 K, and reaction time 7 h, the conversions of phenol and H2O2 and the selectivity for dihydroxybenzene reached 20.4%, 96.9%, and 99.6%, respectively.

Key words: iron, MSU-1 mesoporous molecular sieve, phenol, hydroxylation