催化学报

催化学报 ›› 2015, Vol. 36 ›› Issue (10): 1719-1725.DOI: 10.1016/S1872-2067(15)60908-1

• 论文 • 上一篇    下一篇

主(脱铝Y分子筛纳米腔)-客(Co,Mn和Cox/Mnx三核金属簇合物)纳米复合物催化剂高效催化环己烯环氧化反应

Maryam Moosavifara, Alieh Navid Arbata,b, Zolfaghar Rezvanic, Kamellia Nejatib   

  1. a 马拉盖大学理学院化学系, 马拉盖55181-83111, 伊朗;
    b 帕亚莫努尔大学化学系, 德黑兰19395-3697, 伊朗;
    c Azarbaijan Shahid Madani大学基础科学学院化学系, 大不里士, 伊朗
  • 收稿日期:2015-04-04 修回日期:2015-05-19 出版日期:2015-09-26 发布日期:2015-09-26
  • 通讯作者: Maryam Moosavifar.电话: +98-413-7273068; 传真: +98-413-7276060; 电子信箱: m.moosavifar90@gmail.com, moosavifar@maragheh.ac.ir

Host (dealuminated Y zeolite)-guest (trinuclear metal clusters of Co, Mn and Cox/Mny) as nanocomposite catalysts for the epoxidation of cyclohexene

Maryam Moosavifara, Alieh Navid Arbata,b, Zolfaghar Rezvanic, Kamellia Nejatib   

  1. a Department of Chemistry, Faculty of Science, University of Maragheh, Maragheh, Iran;
    b Department of Chemistry, Payame Noor University, P.O. BOX 19395-3697, Tehran, Iran;
    c Department of Chemistry, Faculty of Basic Sciences, Azarbaijan Shahid Madani University, Tabriz, Iran
  • Received:2015-04-04 Revised:2015-05-19 Online:2015-09-26 Published:2015-09-26

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摘要：

采用模板合成法制备了在脱铝Y分子筛纳米腔中含有Co, Mn, 和Co/Mn混合物的三核金属簇合物的复合物催化剂, 包括[Mn3(O)(CH3COO)6-(py)3]-Y, [Co3(O)(CH3COO)6-(py)3], [Co2Mn(O)(CH3COO)6-(py)3]-Y和[CoMn2(O)(CH3COO)6-(py)3]-Y], 并运用傅里叶变换红外光谱、紫外-可见光光谱、前场扫描电镜、X射线衍射和原子吸收光谱对其进行了表征. 包裹的金属簇合物在环己烯环氧化反应中表现出较高的催化活性, 反应以H2O2/O2为氧化剂, 在加热机械搅拌下进行, 所得环氧化物产率在82.5%-90.7%. 在该催化体系中, NaBr用作氧化助剂可以提高反应性能. 在所制多相催化体系中, 含单核的金属簇合物催化活性更高, 其中以Mn3(O)-DAZY化合物的效率最高. 各催化剂活性顺序为Mn3(O)-DAZY > Co3(O)-DAZY > Mn2Co(O)-DAZY > MnCo2(O)-DAZY.

关键词: 环己烯, 环氧化, 金属簇合物, 脱铝Y分子筛, 钴

Abstract:

Trinuclear metal clusters of Co, Mn and mixtures of Co/Mn including [Mn3(O)(CH3COO)6-(py)3]-Y, [Co3(O)(CH3COO)6-(py)3], [Co2Mn(O)(CH3COO)6-(py)3]-Y and [CoMn2(O)(CH3COO)6-(py)3]-Y] were prepared inside the nanocage of dealuminated Y zeolite by the template synthesis method. These catalysts were characterized by Fourier transform infrared, Ultraviolet-visible, field scanning electron microscopy, X-ray diffraction and atomic absorption spectroscopy. The encapsulated metal clusters showed good catalytic activity in the epoxidation of cyclohexene with H2O2/O2. Epoxide yields were 82.5% to 90.7%. NaBr was used as a promoter for the oxidation. The homonuclear metal clusters showed higher catalytic activity than the others and the highest efficiency was with the Mn3(O)-DAZY compound. The catalytic activity order was Mn3(O)-DAZY > Co3(O)-DAZY > Mn2Co(O)-DAZY > MnCo2(O)-DAZY.

Key words: Cyclohexene, Epoxide, Metal clusters, Dealuminated Y Zeolite, Cobalt