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机构地区:[1]长江大学化学与环境工程学院,湖北荆州434023
出 处:《精细石油化工》2014年第1期28-33,共6页Speciality Petrochemicals
基 金:长江大学博士科研启动基金项目(2012年)
摘 要:采用Fe-TS-1为催化剂,过氧化氢为氧化剂,以1-己烯环氧化为原料合成了1,2-环氧己烷。考察了Fe含量、溶剂、过氧化氢用量、温度、催化剂用量以及反应时间对反应的影响,较优化的反应条件为:n(SiO2)∶n(Fe2O3)=860,溶剂乙腈,反应温度343K,过氧化氢用量0.8mol/L,催化剂用量10.7g/L,反应时间5h。在优化的条件下,过氧化氢的转化率为49.6%,过氧化氢的选择性为68.1%,1-己烯的转化率为33.4%,1,2-环氧己烷的选择性为92.0%,1,2-己二醇的选择性为8.0%。采用甲醇为溶剂时,Fe-TS-1表现出较低的催化活性和选择性;而采用乙腈为溶剂时,Fe-TS-1表现出较高的催化活性和选择性。说明掺杂Fe3+后,TS-1的疏水性发生了改变,乙腈溶剂的采用可能改变了反应的历程。Epoxidation of 1-hexene to 1,2-epoxyhexane over Fe-TS-1 using dilute H2O2 was studied.The effects of Fe content,solvent,reaction temperature,H2O2 concentration,catalyst concentration and reaction time on the epoxidation of 1-hexene were investigated.The optimum reaction conditions were as follows:n(SiO2) ∶ n(Fe2O3) =860,acetonitrile as solvent,reaction temperature was 343 K,H2O2 concentration was 0.8 mol/L,catalyst concentration was 10.7 g/L and reaction time was 5 h.Under the optimum conditions,the H2O2 conversion,H2O2 selectivity,1-hexene conversion,1,2-epoxyhexane and 1,2-hexanediol selectivity were 49.6%,68.1%,33.4%,92.0% and 8.0%,respectively.The catalyst showed low catalytic activity and selectivity when methanol was used as a solvent,while it showed higher catalytic activity and selectivity when acetonitrile was used as the solvent.This effect was due to the changes in the hydrophobic character of TS-1 caused by the incorporation of Fe3+,which might alter the reaction pathway when acetonitrile was used as the solvent.
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