期刊
JOURNAL OF CATALYSIS
卷 294, 期 -, 页码 99-112出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2012.07.008
关键词
N2O direct decomposition; Density functional theory; Beta zeolite; Microkinetic; Mechanism
资金
- National Natural Science Foundation of China [20977004, 21177008, 21121064]
- New Century Program for Excellent Talents in University [NCET-10-0204]
Catalytic activities of M (Fe, Cu, Co)-beta (BEA) zeolites for N2O direct decomposition were systematically investigated by employing both experimental and theoretical [density functional theory (DFT)] approaches. The activities of M-BEA determined by intrinsic kinetic evaluations are in good agreement with the DFT calculations and the microkinetic analyses, revealing that the distinguishing activities of M-BEA were mainly attributed to their distinct energy barriers for the O-2 desorption (Part 3). During the DFT calculations, a unique intermediate (IM) was generated only over Co-BEA, which was verified by the activity evaluation and N2O-TPD experiments, showing that the formation of IM reduced N2O decomposition rate of Co-BEA. The negative effect of the IM was thereafter investigated by the microkinetic analyses through which it was known that the second forward reaction rate constant of Co-BEA was lower than its reverse reaction rate constant, resulting in a final decline of the N2O decomposition rate. (C) 2012 Elsevier Inc. All rights reserved.
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