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Theoretical Study of N 2 O Reduction by CO in Fe‐BEA Zeolite
Author(s) -
Fischer Gerd,
Goursot Annick,
Coq Bernard,
Delahay Gérard,
Pal Sourav
Publication year - 2006
Publication title -
chemphyschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.016
H-Index - 140
eISSN - 1439-7641
pISSN - 1439-4235
DOI - 10.1002/cphc.200600228
Subject(s) - zeolite , chemistry , decomposition , catalysis , molecule , activation energy , cluster (spacecraft) , reduction (mathematics) , computational chemistry , thermodynamics , physics , organic chemistry , geometry , mathematics , computer science , programming language
Quantum mechanical (QM) and QM/molecular mechanics (MM) studies of the full catalytic cycle of N 2 O reduction by CO in Fe‐BEA zeolite, that is, oxidation of BEA‐Fe by N 2 O and reduction of BEA‐Fe‐αO by CO, is presented. A large QM cluster, representing half of the channel of the BEA zeolite, is used. The contribution of the MM embedding to the calculated activation energies is found to be negligible. The minimum‐energy paths for N 2 O decomposition and reduction with CO are calculated using the nudged elastic band (NEB) method. Calculated and experimental activation energies are in good agreement. The two possible orientations for the gaseous molecules adsorbing on the Fe site that are found lead to different activation energies.