钛硅分子筛的制备、表征及其催化丙烯环氧化工艺的研究

石油炼制与化工 ›› 2013, Vol. 44 ›› Issue (6): 59-63.

钛硅分子筛的制备、表征及其催化丙烯环氧化工艺的研究

阳辉¹,靳鹏^1,2,郑晓广^1,2,王向宇¹

1. 郑州大学化学与分子工程学院
2. 中国平煤神马集团能源与化工研究院

收稿日期:2012-10-10 修回日期:2012-11-11 出版日期:2013-06-12 发布日期:2013-05-24
通讯作者: 王向宇 E-mail:xiangyuwang@zzu.edu.cn

PREPARATION OF TITANIUM SILICALITE, CHARACTERIZATION AND ITS APPLICATION IN PROPYLENE EPOXIDATION WITH HYDROGEN PEROXIDE

Received:2012-10-10 Revised:2012-11-11 Online:2013-06-12 Published:2013-05-24

摘要/Abstract

摘要： 以正硅酸乙酯为硅源、钛酸四丁酯为钛源、四丙基氢氧化铵为模板剂，采用水热合成法制备钛硅分子筛。利用X射线粉末衍射（XRD）、紫外-可见吸收光谱（UV-Vis）和扫描电镜（SEM）方法对该分子筛进行了表征。以H2O2为氧化剂、甲醇为溶剂，在淤浆床反应器中研究了钛硅分子筛催化丙烯环氧化反应的性能。结果表明，在钛硅分子筛用量1.5 g、甲醇用量150 mL、30% H2O2 用量25 mL、2.5% NaHCO3用量0.2 mL、反应温度55 ℃、反应压力0.2 MPa、反应时间1 h、丙烯流量 1 L/min的条件下，H2O2的转化率和有效利用率分别达到94.4%和88.8%，环氧丙烷选择性和收率分别为98.7%和87.6%，反应体系中丙烯质量分数约为8.0%。

Abstract: Titanium silicalite was hydrothermally synthesized with tetraethyl orthosilicate, tetrabutyl titanate and tetrapropyl ammonium hydroxide template. The structures of titanium silicalite were characterized by XRD, UV-Vis and TEM. The characterization results indicate that the samples prepared possess MFI structure and good crystallinity, and no non-frame anatase type TiO2 is found. The performance of catalytic epoxidation of propylene by titanium silicalite was studied in a slurry bed reactor using hydrogen peroxide as oxidant and methanol as solvent. Under the optimized conditions (1.5 g titanium silicalite, 150 mL methanol, 25 mL 30% H2O2, 0.2 mL 2.5% NaHCO3, propylene flow 1 L/min, at 0.2 MPa and 55 °C，reaction time of 1 h), the selectivity and yield of propylene oxide are 98.7%, 87.6%, respectively.

阳辉靳鹏郑晓广王向宇. 钛硅分子筛的制备、表征及其催化丙烯环氧化工艺的研究[J]. 石油炼制与化工, 2013, 44(6): 59-63.