The effect of oxidation of ethane to oxygenates on Pt-and Zn-containing LTA zeolites with tunable selectivity  

作　　者：Baoyu Liu Su Cheun Oh Huiyong Chen Dongxia Liu 

机构地区：[1]School of Chemical Engineering and Light Industry, Guangdong University of Technology [2]Department of Chemical and Biomolecular Engineering, University of Maryland, College Park [3]School of Chemical Engineering, Northwest University

出　　处：《Journal of Energy Chemistry》2019年第3期42-48,共7页能源化学（英文版）

基　　金：support from the National Science Foundation(NSF-CBET-1264599 and 1351384);support of the Maryland NanoCenter and its NispLab;supported in part by the NSF as a MRSEC Shared Experimental Facility;the China Scholarship Council (CSC) (No. 201306150076) for a fellowship to support his study at the University of Maryland

摘　　要：Platinum and zinc containing LTA zeolite catalysts with tunable meso/microporosity were prepared by using ligand-metal precursors under hydrothermal condition. These materials were employed for oxidation of ethane to oxygenates using hydrogen peroxides as oxidant under mild reaction condition. The results showed that platinum and zinc loaded LTA zeolites were effective for the partial oxidation of ethane with hydrogen peroxide giving the desired C_2 oxygenates. Moreover, the C_1 oxygenates were also obtained through subsequent C–C bond scission pathways. The over oxidation of ethanol/methanol to acetic acid/formic acid could be inhibited through the introduction of mesoporosity in LTA zeolites. Our findings for oxidation of ethane suggested that the selectivity to the oxidation products such as alcohols and acids could be tailored by tuning the metal species within the LTA zeolites and porosity of catalysts, indicating that a balance between the meso/microporosity and metal species in LTA zeolites can be realized for desirable catalysis by one-pot synthesis of zeolites. In addition, the selectivity to oxygenates can also be tuned by control of the reaction conditions, i.e. concentration of hydrogen peroxide or reaction time.Platinum and zinc containing LTA zeolite catalysts with tunable meso/microporosity were prepared by using ligand-metal precursors under hydrothermal condition. These materials were employed for oxidation of ethane to oxygenates using hydrogen peroxides as oxidant under mild reaction condition. The results showed that platinum and zinc loaded LTA zeolites were effective for the partial oxidation of ethane with hydrogen peroxide giving the desired C_2 oxygenates. Moreover, the C_1 oxygenates were also obtained through subsequent C–C bond scission pathways. The over oxidation of ethanol/methanol to acetic acid/formic acid could be inhibited through the introduction of mesoporosity in LTA zeolites. Our findings for oxidation of ethane suggested that the selectivity to the oxidation products such as alcohols and acids could be tailored by tuning the metal species within the LTA zeolites and porosity of catalysts, indicating that a balance between the meso/microporosity and metal species in LTA zeolites can be realized for desirable catalysis by one-pot synthesis of zeolites. In addition, the selectivity to oxygenates can also be tuned by control of the reaction conditions, i.e. concentration of hydrogen peroxide or reaction time.

关 键 词：ZEOLITE Hierarchical ETHANE Porosity 

分 类 号：O4[理学—物理]