用负载于中孔分子筛的钯催化剂合成碳酸二乙酯  

Preparation of Diethyl Carbonate over Palladium Catalysts Supported on Mesoporous Molecular Sieve

作　　者：苏跃华[1] 姜玄珍[2] 

机构地区：[1]陕西师范大学化学与材料科学学院,西安710062 [2]浙江大学化学系

出　　处：《应用化学》2002年第10期994-997,共4页Chinese Journal of Applied Chemistry

摘　　要：利用微分反应器研究了连续流动床反应器中负载型钯催化剂对反应 CO+C2 H5ONO的催化活性 ,催化剂采用粉末状的 Si-MCM-41 (Si M)和 Ti-MCM-41 (Ti M)与相应的金属溶液逐滴浸渍而成 ;结果表明 ,铜和钛作为添加剂可增加碳酸二乙酯 (DEC)和草酸二乙酯 (DEO)的产率。负载于 Si M上的催化剂比负载于Ti M的催化剂表现出较高的活性 ,它表明载体特性在催化反应中确实起着关键作用。 2种添加剂即钛和铜对催化行为表现出不同的作用 :以 Si M为载体时 ,添加剂铜有利于 DEO的形成 ,添加剂 Ti有利于 DEC形成 ;然而 ,以 Ti M为载体的情况下 ,2种添加剂表现出以 Si M为载体相反的趋向 ,这些表明在反应 CO +C2 H5ONO中存在催化剂上的载体和金属组分协同催化。需进一步研究碳酸二乙酯的新法合成中添加剂和载体的作用。The catalytic activities of supported palladium catalysts for the synthesis of diethyl carbonate (DEC) in vapor phase have been studied in a fixed bed reactor. The catalysts were prepared by impregnating Si MCM 41(SiM) and Ti MCM 41(TiM) powder in corresponding solution of PdCl 2 , CuCl 2·2H 2O and (C 4H 9O) 4Ti. The results revealed that addition of copper and titanium increased the yields of both DEC and diethyl oxalate(DEO). The catalytic activity of the catalysts supported on SiM was higher than that of the catalysts supported on TiM. Copper and titanium function differently in on the catalyts: with SiM as support, Cu was in favorable of DEO formation, while Ti is of DEC formation. In the case of TiM as support, however, two additives showed opposite results. The above results suggested the support and the additive have synergistic action on the reaction of CO with C 2H 5ONO.

关 键 词：中孔分子筛 碳酸二乙酯 草酸二乙酯 羰基化 钯 负载型催化剂 催化合成 

分 类 号：O623.662[理学—有机化学] O643.36[理学—化学]