Liquid phase propylene epoxidation with H2O2 on TS-1/SiO2 catalyst in a fixed-bed reactor: experiments and deactivation kinetics

被引:11
作者
Feng, Wenping [1 ]
Wang, Yaquan [1 ]
Wu, Guoqiang [1 ]
Lin, Yi [1 ]
Xu, Juan [1 ]
Shi, Hainan [1 ]
Zhang, Teng [1 ]
Wang, Shuhai [1 ]
Wu, Xiaoxue [1 ]
Yao, Pengxu [1 ]
机构
[1] Tianjin Univ, Sch Chem Engn & Technol, Key Lab Green Chem Technol, Minist Educ, Tianjin 300072, PR, Peoples R China
关键词
Heterogeneous Catalysis; Kinetics; Oxidation; Zeolites; HYDROGEN-PEROXIDE; TITANIUM SILICALITE; TS-1; CATALYST; REGENERATION; PROPENE; OXIDE; HYDROXYLATION; OXIDATION; OLEFINS; PHENOL;
D O I
10.1002/jctb.4462
中图分类号
Q81 [生物工程学(生物技术)]; Q93 [微生物学];
学科分类号
071005 ; 0836 ; 090102 ; 100705 ;
摘要
BACKGROUNDThe epoxidation of propylene with H2O2 in liquid phase catalyzed by a TS-1/SiO2 catalyst in a fixed-bed reactor has been studied. The effects of reaction temperature (313-328 K), methanol concentrations (55-70 wt%) and hydrogen peroxide concentrations (9-15 wt%) on the reaction are investigated. The fresh, deactivated and regenerated catalysts were characterized with XRD, FT-IR, UV-vis, N-2 sorption and TG to study the reasons for catalyst deactivation. In addition, the kinetics of catalyst deactivation was studied by fitting the experimental data. RESULTSThe rate of decrease of H2O2 conversion decreases with increasing reaction temperature and methanol concentration, but increases with increasing hydrogen peroxide concentration. The reason for catalyst deactivation is that the bulky organic matter covers the active centers. The study on deactivation kinetics shows that the deactivation reaction order is 2, and an expression for H2O2 conversion as a function of reaction time is obtained. CONCLUSIONThe operating conditions such as reaction temperature, methanol concentration and hydrogen peroxide concentration remarkably affect the reaction. The kinetic parameters including deactivation reaction order and activation energy are developed by fitting the experimental data based on the Wojciechowski model. (c) 2014 Society of Chemical Industry
引用
收藏
页码:1489 / 1496
页数:8
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