溶剂对TS-1催化丙烯环氧化反应的影响  

Effect of solvents on propylene epoxidation with the TS-1 catalyst

作　　者：吴玉龙[1] 刘青山[1] 苏雪丽[2] 米镇涛[2] 

机构地区：[1]清华大学核能与新能源技术研究院,北京100084 [2]天津大学化工学院,天津300072

出　　处：《清华大学学报（自然科学版）》2007年第9期1511-1515,共5页Journal of Tsinghua University(Science and Technology)

基　　金：国家自然科学基金资助项目(20506011);国家"九七三"重点基础研究项目(200048005)

摘　　要：溶剂对钛硅分子筛TS-1催化丙烯环氧化反应具有重要影响。该文对甲醇、异丙醇和仲丁醇3种醇溶剂及丙酮、乙腈和四氢呋喃等有机溶剂中环氧化反应活性进行了研究,实验结果活性顺序为:甲醇>异丙醇>仲丁醇>乙腈>丙酮>四氢呋喃。以催化反应机理为基础,通过电子效应、空间位阻效应、溶剂极性、物理扩散和分配、溶剂氧化副反应、环氧丙烷(PO)醚化副反应、催化剂失活和丙烯溶解度等多种因素分析了溶剂对环氧化反应的影响。电子效应、空间位阻效应和溶剂极性是影响反应的重要因素,研究工作为今后同类反应溶剂的选取提供理论根据和指导,为PO清洁生产工艺的进一步工业化奠定基础。Solvents have an important effect on the epoxidation of propylene catalyzed by TS-1. Experimental results show that the catalytic epoxidation activity of various solvents can be ranked as： methanol 〉 2-propanol 〉 2-butanol 〉 acetonitrile 〉 acetone tetrahydrofuran. The reaction mechanism was analyzed to study the effects of the solvents on the epoxidation in terms of the electronic effect, the steric effect, the solvent polarity, the effect of solvent on sorption and reactant diffusion, the alcohol oxidation, the etherization of PO, the deactivation of TS-1 and the propylene solubility in the solvents. The electronic effect, steric effect, and solvent polarity were the main effects. This work provides a basis for choosing solvents for these reactions for further industrialization.

关 键 词：钛硅分子筛 丙烯 环氧化反应 溶剂效应 

分 类 号：O643.132[理学—物理化学]