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American Chemical Society, Journal of Physical Chemistry C, 8(119), p. 4224-4234, 2015

DOI: 10.1021/jp5126975

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In Situ Characterization of Highly Dispersed, Ceria-Supported Fe Sites for NO Reduction by CO

This paper is available in a repository.
This paper is available in a repository.

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Abstract

Highly dispersed FeOx was impregnated onto CeO2 using the unique precursor Na/Fe-ethylenediaminetetraacetate (NaFeEDTA) at varying Fe surface density (0-1.5 Fe/nm2). These catalysts were used for NO reduction by CO, and were compared to a more traditional Fe(NO3)3 precursor impregnated on Na-promoted CeO2. Extensive characterization and spectroscopic measurements showed that NaFeEDTA produced a narrower distribution of smaller, non-crystalline, surface FeOx species with excellent redox cyclability (Fe3+↔Fe2+). The NaFeEDTA catalysts exhibited corresponding higher steady-state activity for NO reduction by CO. In situ x-ray absorption spectroscopy with simultaneous gas phase monitoring indicated that NO conversion began concurrent with reduction of Fe and Ce, suggesting that NO reduction occurred at a reduced Fe-O-Ce interface site. These results illustrate a new synthesis-structure-activity relationship for NO reduction by CO over redox-cycling FeOx sites that may support future rational design of emission control catalysts without Pt-group metals or zeolites.