INVESTIGATION OF THE REACTION PATHWAYS IN SELECTIVE CATALYTIC REDUCTION OF NO WITH NH3 OVER V2O5 CATALYSTS - ISOTOPIC LABELING STUDIES USING O-18(2), (NH3)-N-15, (NO)-N-15, AND (NO1)-N-15-O-18

被引:89
|
作者
OZKAN, US
CAI, YP
KUMTHEKAR, MW
机构
[1] Department of Chemical Engineering, Ohio State University, Columbus
[2] Department of Chemical Engineering, Lehigh University, Bethlehem
关键词
D O I
10.1006/jcat.1994.1306
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
Isotopic tracer studies were performed to investigate the reaction network of selective catalytic reduction of nitric oxide over vanadia catalysts having preferential exposure of different crystal planes. The catalysts were characterized using BET surface area analysis, X-ray diffraction, laser Raman spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, 3-D imaging, and thermal analysis techniques. The product analysis was carried out by a combination of chemiluminescence NOx analysis, gas chromatography-mass spectrometry, and chemical titration methods. The isotopic labeling experiments were performed under steady-state reaction conditions by using NH3 + NO + O-16(2) --> NH3 + NO + O-18(2), (NH3)-N-14 + NO + O-2 --> (NH3)-N-15 + NO + O-2, NH3 + (NO)-N-14 + O-2 --> NH3 + (NO)-N-15 + O-2, and NH3 + (NO)-N-14-O-16 + O-16(2) --> NH3 + (NO)-N-15-O-18 + O-18(2) switches. Interaction of NO with the vanadia surface was also studied using a (NO)-N-14-O-16 --> (NO)-N-15-O-18 switch. The results obtained in these experiments were combined with the tracer studies performed in ammonia oxidation reactions over the same catalysts to elucidate the reaction pathways involved in SCR reactions, to compare the surface residence times of nitrogen containing species, as well as to quantify the role of ammonia oxidation in SCR reactions. (C) 1994 Academic Press, Inc.
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页码:390 / 403
页数:14
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