Three-Dimensionally Ordered Macroporous La0.6Sr0.4MnO3 Supported Ag Nanoparticles for the Combustion of Methane

被引:97
作者
Arandiyan, Hamidreza [1 ]
Dai, Hongxing [2 ]
Deng, Jiguang [2 ]
Wang, Yuan [2 ,3 ]
Sun, Hongyu [4 ]
Xie, Shaohua [2 ]
Bai, Bingyang [1 ]
Liu, Yuxi [2 ]
Ji, Kemeng [2 ]
Li, Junhua [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
[2] Beijing Univ Technol, Lab Catalysis Chem & Nanosci, Dept Chem & Chem Engn, Coll Environm & Energy Engn, Beijing 100124, Peoples R China
[3] Natl Res Ctr Geoanal, Beijing 100037, Peoples R China
[4] Tsinghua Univ, Beijing Natl Ctr Elect Microscopy, State Key Lab New Ceram & Fine Proc, Sch Mat Sci & Engn,Key Lab Adv Mat MOE, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
PMMA-TEMPLATING PREPARATION; HIGH CATALYTIC PERFORMANCE; HIGH-SURFACE-AREA; CARBON-MONOXIDE; TOTAL OXIDATION; CO OXIDATION; METAL-OXIDES; LAMNO3; PEROVSKITE; GOLD;
D O I
10.1021/jp502256t
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
A series of Ag nanoparticles (NPs) supported on three-dimensionally ordered macroporous (3DOM) La0.6Sr0.4MnO3 (yAg/3DOM La0.6Sr0.4MnO3; y = 0, 1.57, 3.63, and 5.71 wt %) were successfully prepared with high surface areas (38.2-42.7 m(2)/g) by a facile novel reduction method using poly methacrylate colloidal crystal as template in a dimethoxytetraethylene glycol (DMOTEG) solution. Physicochemical properties of these materials were characterized by means of numerous techniques, and their catalytic activities were evaluated for the combustion of methane. It is shown that the yAg/3DOM La0.6Sr0.4MnO3 materials possessed unique nanovoid-like 3DOM architectures, and the Ag NPs were well dispersed on the inner walls of macropores. Among the La1-xSrxMnO3 (x = 0.2, 0.4, 0.6, 0.8) and yAg/3DOM La0.6Sr0.4MnO3 (y = 0, 1.57, 3.63, and 5.71 wt %) samples, 3.63 wt % Ag/3DOM La0.6Sr0.4MnO3 performed the best, giving T-10%, T-50%, and T-90% (temperatures corresponding to methane conversion =10, 50, and 90%) of 361, 454, and 524 degrees C, respectively, and the highest turnover frequency (TOFAg) value of 1.86 x 10(-5) (mol/mol(Ag) s) at 300 degrees C. The apparent activation energies (39.1-37.5 kJ/mol) of the yAg/3DOM La0.6Sr0.4MnO3 samples were much lower than that (91.4 kJ/mol) of the bulk La0.6Sr0.4MnO3 sample. The effects of water vapor and sulfur dioxide on the catalytic activity of the 3.63 wt % Ag/3DOM La0.6Sr0.4MnO3 sample were also examined. It is concluded that its super catalytic activity was associated with its high oxygen adspecies concentration, good low-temperature reducibility, large surface area, and strong interaction between Ag and La0.6Sr0.4MnO3 as well as the unique nanovoid-walled 3DOM structure.
引用
收藏
页码:14913 / 14928
页数:16
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