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

doi:10.1021/jp5126975

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

Northwestern University

Research output: Contribution to journal › Article

18 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 language	English
Pages (from-to)	4224-4234
Number of pages	11
Journal	Journal of Physical Chemistry C
Volume	119
Issue number	8
DOIs	https://doi.org/10.1021/jp5126975
Publication status	Published - Feb 26 2015

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ASJC Scopus subject areas

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

Cite this

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

In situ characterization of highly dispersed, ceria-supported fe sites for no reduction by CO. / Roberts, Charles A.; Prieto-Centurion, Dario; Nagai, Yasutaka; Nishimura, Yusaku F.; Desautels, Ryan D.; Van Lierop, Johan; Fanson, Paul T.; Notestein, Justin M.

In: Journal of Physical Chemistry C, Vol. 119, No. 8, 26.02.2015, p. 4224-4234.

Research output: Contribution to journal › Article

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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, 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.",

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AU - Prieto-Centurion, Dario

AU - Nagai, Yasutaka

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AU - Desautels, Ryan D.

AU - Van Lierop, Johan

AU - Fanson, Paul T.

AU - Notestein, Justin M.

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N2 - 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.

AB - 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.

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10.1021/jp5126975