主(脱铝Y分子筛纳米腔)-客(Co,Mn和Co_x/Mn_x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(英文)  

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

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作  者:Maryam Moosavifar Alieh Navid Arbat Zolfaghar Rezvani Kamellia Nejati 

机构地区:[1]马拉盖大学理学院化学系,伊朗马拉盖55181-83111 [2]帕亚莫努尔大学化学系,伊朗德黑兰19395-3697 [3]Azarbaijan Shahid Madani大学基础科学学院化学系,伊朗大不里士

出  处:《催化学报》2015年第10期1719-1725,共7页

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[CoM n2(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,Na Br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?MnC o2(O)-DAZY.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 elec-tron 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.

关 键 词:环己烯 环氧化 金属簇合物 脱铝Y分子筛  

分 类 号:O643.36[理学—物理化学] TB33[理学—化学]

 

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