引用本文:
苏跃华, 姜玄珍. 用负载于中孔分子筛的钯催化剂合成碳酸二乙酯[J]. 应用化学,
2002, 19(10): 994-997.
Citation: SU Yue-Hua, JIANG Xuan-Zhen. Preparation of Diethyl Carbonate over Palladium Catalysts Supported on Mesoporous Molecular Sieve[J]. Chinese Journal of Applied Chemistry, 2002, 19(10): 994-997.
Citation: SU Yue-Hua, JIANG Xuan-Zhen. Preparation of Diethyl Carbonate over Palladium Catalysts Supported on Mesoporous Molecular Sieve[J]. Chinese Journal of Applied Chemistry, 2002, 19(10): 994-997.
用负载于中孔分子筛的钯催化剂合成碳酸二乙酯
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+C2H5ONO的催化活性,催化剂采用粉末状的Si-MCM-41(SiM)和Ti-MCM-41(TiM)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SiM上的催化剂比负载于TiM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SiM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TiM为载体的情况下,2种添加剂表现出以SiM为载体相反的趋向,这些表明在反应CO+C2H5ONO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。
English
Preparation of Diethyl Carbonate over Palladium Catalysts Supported on Mesoporous Molecular Sieve
Abstract:
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 PdCl2, CuCl2·2H2O and (C4H9O)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 C2H5ONO.
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Key words:
- diethyl carbonate
- / diethyl oxalate
- / carbonylation
- / supported palladium catalyst
- / copper
- / titanium
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