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Mechanism of CO Disproportionation on Reduced Ceria
Author(s) -
Liu Yi,
Wen Cun,
Guo Yun,
Liu Xiaohui,
Ren Jiawen,
Lu Guanzhong,
Wang Yanqin
Publication year - 2010
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.200900246
Subject(s) - disproportionation , chemistry , radical disproportionation , dissociation (chemistry) , photochemistry , catalysis , unpaired electron , electron paramagnetic resonance , bond cleavage , molecule , inorganic chemistry , infrared spectroscopy , organic chemistry , nuclear magnetic resonance , physics
CO disproportionation produces carbon deposits that cover active sites and induce catalyst deactivation. However, understanding of this detrimental reaction on reduced ceria is deficient. Herein, the reversibility and reaction mechanism of CO disproportionation on reduced ceria are investigated. The reversibility of the CO disproportionation was studied by CO pulse, isotopic oxygen tracer, thermal analysis, and CO 2 pulse experiments. In situ diffuse‐reflectance infrared Fourier transform spectra indicate that the CO bond of the CO molecule on Ce 3+ ion is weakened. With CO bond dissociation, asymmetrical inorganic carboxylate species are formed. These species are the key reaction intermediates in CO disproportionation and are further converted to produce CO 2 . EPR experiments indicate that the unpaired electrons produced by the reduction weaken the CO bond through back‐donation of electrons.