Catalytic reduction of NO with H2 over redox-cycling Fe on CeO2

Dario Prieto-Centurion, Todd R. Eaton, Charles A. Roberts, Paul T. Fanson, Justin M Notestein

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

Removal of NOx species from automotive emissions continues to be a challenge, particularly using replacements for Pt-group metals. Here, we demonstrate the synthesis of FeOx domains on CeO2 from the precursor Fe ethylenediaminetetraacetate (NaFeEDTA) and its utility in the reduction of NO with H2 as a model reaction for tailpipe emissions. Diffuse-reflectance UV-visible and X-ray absorption near-edge spectroscopies indicate the formation of small, non-crystalline FeOx domains. Using the EDTA precursor, TPR and in situ XANES show that up to 45% of the FeOx centers were capable of undergoing redox cycles in H2 up to 550°C, whereas only 23% of FeOx centers derived from Fe(NO3)3 were redox active. Similarly, at comparable Fe surface densities, the FeEDTA-derived catalysts were more active than the nitrate-derived materials in the reduction of NO to N2 (85-95% selectivity) with H2 at 450°C. The presence of both the bulky organic ligand and the alkali is essential for the observed enhancements in fraction redox active and to achieve high NO reduction rates. Rates over all materials were fit to a single correlation against the number of redox-active FeOx centers, suggesting that these are the catalytic active sites. The new materials describe here may offer new avenues for emissions control without Pt-group metals or substituted zeolites.

Original languageEnglish
Pages (from-to)68-76
Number of pages9
JournalApplied Catalysis B: Environmental
Volume168-169
DOIs
Publication statusPublished - Jun 1 2015

Fingerprint

Metals
metal
emission control
EDTA
Zeolites
ligand
Emission control
reflectance
Ethylenediaminetetraacetic acid
X ray absorption
Alkalies
replacement
catalyst
spectroscopy
Edetic Acid
Nitrates
nitrate
Ligands
Spectroscopy
Catalysts

Keywords

  • Ceria
  • DeNO
  • Emissions
  • Redox
  • XANES

ASJC Scopus subject areas

  • Catalysis
  • Process Chemistry and Technology
  • Environmental Science(all)

Cite this

Catalytic reduction of NO with H2 over redox-cycling Fe on CeO2. / Prieto-Centurion, Dario; Eaton, Todd R.; Roberts, Charles A.; Fanson, Paul T.; Notestein, Justin M.

In: Applied Catalysis B: Environmental, Vol. 168-169, 01.06.2015, p. 68-76.

Research output: Contribution to journalArticle

Prieto-Centurion, Dario ; Eaton, Todd R. ; Roberts, Charles A. ; Fanson, Paul T. ; Notestein, Justin M. / Catalytic reduction of NO with H2 over redox-cycling Fe on CeO2. In: Applied Catalysis B: Environmental. 2015 ; Vol. 168-169. pp. 68-76.
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