4.8 Article

Distribution and Valence State of Ru Species on CeO2 Supports: Support Shape Effect and Its Influence on CO Oxidation

Journal

ACS CATALYSIS
Volume 9, Issue 12, Pages 11088-11103

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b03113

Keywords

RuOx/CeO2 catalyst; morphology effect; reduction treatment; oxygen storage capacity; CO oxidation

Funding

  1. National Science Foundation [CHE-1657943, CBET-1856729]
  2. American Chemical Society Petroleum Research Fund [52323]
  3. Alabama Water Institute
  4. Alabama Transportation Institute

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In this work, ruthenium (Ru) catalysts supported on CeO2 nanorods (NR), nanocubes (NC), and nanoctahedra (NO) were comparatively investigated to correlate the shape and exposed surface planes ({100}, {110}, and {111}) of nanoscale CeO2 supports with their low-temperature CO oxidation activity. Within the 5Ru/CeO2-r catalysts with three morphologies after reduction treatment, the Ru supported on CeO2 NR exhibited enhanced low-temperature (<100 degrees C) hydrogen consumption and superior room-temperature CO oxidation activity (similar to 9% CO conversion). Both X-ray photoelectron spectroscopy and X-ray absorption spectroscopy measurements revealed that Run+ homogeneously predominates the 5Ru/CeO2NR-r, which is very different from partial metallic Ru-0 supported on CeO2 NC and NO, indicating the strong metal-support interaction formation between Ru and CeO2 NR by Ru ions diffusing into CeO2 surface lattice or forming Ru-O-Ce bonds at the interface. The enriched surface defects on the exposed {111} planes of CeO2 NR support are believed to be the key to the formation of cationic Ru species, which is of vital importance for the superior room-temperature CO oxidation activity of the 5Ru/CeO2NR-r catalyst. The higher surface oxygen vacancy concentration on 5Ru/CeO2NR-r than those on the CeO2 NC and NO is also crucial for adsorption/dissociation of oxygen in achieving low-temperature CO oxidation activity.

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