期刊
CHINESE JOURNAL OF CATALYSIS
卷 35, 期 8, 页码 1289-1298出版社
SCIENCE PRESS
DOI: 10.1016/S1872-2067(14)60154-6
关键词
Selective catalytic reduction; Nitrogen oxide; Ammonia; Amorphous Ce-Ti mixed oxide; In situ infrared; Mechanism
资金
- National Natural Science Foundation of China [21277060, 21107030]
- Development Program of the Science and Technology of Shandong Province [2011GSF11702]
- Foundation for Outstanding Young Scientist in Shandong Province [BS2011HZ002]
- Natural Science Foundation of Shandong Province [ZR2013BQ003]
- Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control of Nanjing University of Information Science and Technology [KHK1116]
- Jiangsu Province Innovation Platform for Superiority Subject of Environmental Science and Engineering
A series of in situ infrared (IR) studies of the selective catalytic reduction (SCR) of NOx with NH3 on the short-range ordered structure Ce-O-Ti sites in amorphous Ce-Ti mixed oxides were performed. Under the reaction conditions, the catalyst surface was mainly covered by NH3 ad-species and no NOx ad-species were detected. The reaction order of 0.5-0.6 with respect to NO confirmed a hybrid Langmuir-Hinshelwood and Eley-Rideal mechanism. A possible route may involve the reaction of NH3 ad-species and weakly adsorbed NOx to form an active intermediate, NHyNO3 (y = 0-4); this was confirmed by GAUSSIAN calculations and the in situ IR results. The Ce-O-Ti structure, with Ce-Ti interactions on the atomic scale, enhanced the redox properties in the active temperature window of the SCR reactions. (C) 2014, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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