Intimate contact of enolic species with silver sites benefits the SCR of NOx by ethanol over Ag/Al2O3

被引:46
作者
Yan, Yong [1 ]
Yu, Yunbo [1 ]
He, Hong [1 ]
Zhao, Jiaojiao [1 ]
机构
[1] Chinese Acad Sci, Ecoenvironm Sci Res Ctr, Beijing 100085, Peoples R China
基金
中国国家自然科学基金;
关键词
Selective catalytic reduction of NOx; Enolic species; Ag/Al2O3; Acetate; Isocyanate; SELECTIVE CATALYTIC-REDUCTION; ALUMINA-SUPPORTED SILVER; LEAN-NOX; FTIR SPECTROSCOPY; HIGHER HYDROCARBONS; MECHANISTIC ASPECTS; DENOX PERFORMANCE; ORGANIC-COMPOUNDS; NITROGEN-OXIDES; ISOCYANATE;
D O I
10.1016/j.jcat.2012.05.021
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
Alumina-supported silver (Ag/Al2O3) catalysts with different silver loadings were investigated for the selective catalytic reduction of NOx by ethanol. The catalytic role of silver in the formation of enolic species was studied by ultraviolet-visible spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy combined with mass spectrometry, density functional theory calculations, and kinetic measurements. It was found that the enolic species originating from the partial oxidation of ethanol over Ag/Al2O3 prefer to adsorb on or close to silver sites, in intimate contact with the active phase. This adsorption behavior of this enolic species contributes to its high activity for the formation of isocyanate species (-NCO) and the final product N-2 during the NOx reduction by ethanol over Ag/Al2O3. Surface acetate also formed during this process, while only interacting with Al sites, resulting in a lower activity for -NCO formation. Meanwhile, the mechanism of the NOx reduction by ethanol was discussed. (C) 2012 Elsevier Inc. All rights reserved.
引用
收藏
页码:13 / 26
页数:14
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