MnOx-CeO2 mixed oxides prepared by co-precipitation for selective catalytic reduction of NO with NH3 at low temperatures

被引:1899
作者
Qi, GS
Yang, RT [1 ]
Chang, R
机构
[1] Univ Michigan, Dept Chem Engn, Ann Arbor, MI 48109 USA
[2] Elect Power Res Inst, Power Generat, Air Pollut Control, Palo Alto, CA 94304 USA
关键词
selective catalytic reduction of NO; low temperature SCR by NH3; Mn-Ce mixed oxide; co-precipitation;
D O I
10.1016/j.apcatb.2004.01.023
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 [物理化学]; 081704 [应用化学];
摘要
A series of manganese-cerium oxide catalysts were prepared by co-precipitation method and used for low temperature selective catalytic reduction (SCR) of NOx with ammonia in the presence of excess O-2. These catalysts were characterized by X-ray diffraction (XRD), surface area measurement and FTIR. The experimental results showed that the best Mn-Ce mixed-oxide catalyst yielded 95% NO conversion at 150degreesC at a space velocity of 42,000 h(-1). As the manganese content was increased from 0 to 40% (i.e. the molar ratio of Mn/(Mn+Ce)), NO conversion increased significantly, but decreased at higher manganese contents. The most active catalyst was obtained with a molar Mn/(Mn + Ce) ratio of 0.4. Only N-2 rather than N2O was found in the product when the temperature was below 150degreesC. At higher temperatures, trace amounts of N2O were detected. A mechanistic pathway for this reaction was proposed based on earlier findings and FTIR results obtained in this work. The initial step was the adsorption of NH3 on Lewis acid sites of catalyst, followed by reaction with nitrite species to produce N-2 and H2O. Possible intermediates are proposed and all the intermediates could transform into NH2NO, which could further react to produce N-2 and H2O. (C) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:93 / 106
页数:14
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