丙氨酸-水杨醛席夫碱锰(Ⅲ)配合物的制备及其对烯烃环氧化的催化性能  

Preparation of Anchored Mn(Ⅲ) Complex from Alanine and Salicylaldehyde and Its Catalytic Performancefor Olefin Epoxidation

作　　者：赵继全[1] 韩建萍[1] 张月成[1] 

机构地区：[1]河北工业大学化工学院,天津300130

出　　处：《催化学报》2005年第7期571-576,共6页

基　　金：国家自然科学基金资助项目(20376017).

摘　　要：丙氨酸与水杨醛反应生成含羧基席夫碱,利用羧基与氨丙基三乙氧基硅烷中的氨基生成酰胺键得到三乙氧基硅官能团化的配体.该配体与乙酸锰配位生成的配合物与正硅酸乙酯通过溶胶凝胶方法共聚制得锚链固定的多相化催化剂.利用FTIR,XPS和N2吸附法对该多相化催化剂进行了表征.与均相催化剂相比,该催化剂对环己烯环氧化反应的催化活性及选择性较高.在环己烯为25mmol,异丁醛为50mmol,催化剂用量为0.01mmol,反应温度为35℃,反应时间为6h的条件下,环己烯转化率可达99.6%,环氧环己烷选择性可达88.2%.循环使用6次后催化剂性能没有明显改变.A ligand with the functional group triethoxysilanyl was prepared by employing the formation of amide bond from the reaction of 3-aminopropyl triethoxysilane with carboxy of a schiff base from the reaction of alanine with salicylaldehyde. This ligand coordinated with Mn(OAc)_2 to give a complex. An anchored and encapsulated catalyst was obtained by the copolymerization of complex with tetraethoxysilane by the sol-gel technique. This heterogenized catalyst was characterized by FT-IR, XPS and N_2 adsorption. The catalyst had higher catalytic activity and selectivity for cyclohexene epoxide than the homogeneous one in the epoxidation of cyclohexene. No catalyst leaching took place during the reaction. Under the conditions of n(Cy-C_6H_ 10 ) =25 mmol, n(i-C_3H_7CHO) =50 mmol, n(cat) =0.01 mmol, θ=35 ℃ and t=6 h, the conversion of cyclohexene and the selectivity for cyclohexene epoxide were 99.6% and 88.2%, respectively. Furthermore, the catalyst performance did not decreased remarkably after 6 recycle runs.

关 键 词：丙氨酸 水杨醛 席夫碱 锰配合物 溶胶-凝胶法 多相化催化剂 环己烯 环氧化 环氧化物 

分 类 号：O643.36[理学—物理化学]