1D-MnO2, 2D-MnO2 and 3D-MnO2 for low-temperature oxidation of ethanol

被引:282
作者
Bai, Bingyang [1 ]
Li, Junhua [1 ]
Hao, Jiming [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
关键词
Mesoporous material; Manganese oxide; Ethanol oxidation; Three-dimensional structure; Hard template; MIXED-OXIDE CATALYSTS; PERFORMANCE; COMBUSTION; FORMALDEHYDE; MANGANESE; SURFACE; COPPER; CO; NANOCRYSTAL; BETA-MNO2;
D O I
10.1016/j.apcatb.2014.08.044
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
1D-MnO2 synthesized using the hydrothermal method was a single-crystal nano-rod with a tetragonal structure. 2D-MnO2 and 3D-MnO2 prepared by the hard template method possess 2D and 3D pore channels, respectively, good pore size distributions and orderly polycrystalline walls due to perfect replication of their templates containing hexagonal (p6mm) pore channel structures and symmetrical cubic (ia3d) structures, respectively. The physicochemical properties of these samples were characterized, and their low-temperature activities for ethanol oxidation were evaluated. 3D-MnO2 exhibited the best catalytic properties for ethanol oxidation due to better low-temperature reducibility and more abundant surface-adsorbed oxygen species and Mn4+ ions. The complete oxidation of ethanol to CO2 was achieved at 150 degrees C on 3D-MnO2. The turnover frequency (TOF) of 3D-MnO2 was the highest (i.e., 0.019 h(-1) at 40 degrees C, 0.047 h(-1) at 70 degrees C and 0.17 h(-1) at 110 degrees C), and its apparent activation energy for the reaction was the lowest (i.e., 28.2 kJ/mol). After the addition of 10 vol.% H2O, the complete oxidation of ethanol to CO2 was obtained at 190 degrees C on 3D-MnO2. There was no obvious decrease after the sample was run for 160 h. The mesoporous MnO2 catalysts, especially 3D-MnO2, are very promising materials for the efficient elimination of ethanol. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码:241 / 250
页数:10
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