In situ characterization of highly dispersed, ceria-supported fe sites for no reduction by CO

Charles A. Roberts, Dario Prieto-Centurion, Yasutaka Nagai, Yusaku F. Nishimura, Ryan D. Desautels, Johan Van Lierop, Paul T. Fanson, Justin M. Notestein

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19 Citations (Scopus)

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, noncrystalline, 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.

Original languageEnglish
Pages (from-to)4224-4234
Number of pages11
JournalJournal of Physical Chemistry C
Volume119
Issue number8
DOIs
Publication statusPublished - Feb 26 2015

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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    Roberts, C. A., Prieto-Centurion, D., Nagai, Y., Nishimura, Y. F., Desautels, R. D., Van Lierop, J., Fanson, P. T., & Notestein, J. M. (2015). In situ characterization of highly dispersed, ceria-supported fe sites for no reduction by CO. Journal of Physical Chemistry C, 119(8), 4224-4234. https://doi.org/10.1021/jp5126975