Co-existence of atomically dispersed Ru and Ce3+ sites is responsible for excellent low temperature N2O reduction activity of Ru/CeO2

Song, Inhak; Wang, Yong; Szanyi, János; Khivantsev, Konstantin

doi:10.1016/j.apcatb.2023.123487

Co-existence of atomically dispersed Ru and Ce³⁺ sites is responsible for excellent low temperature N₂O reduction activity of Ru/CeO₂

Journal Article · Tue Nov 07 04:00:00 EST 2023 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2023.123487· OSTI ID:2395913

Song, Inhak ^[1]; Wang, Yong ^[2]; Szanyi, János ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Institute for Integrated Catalysis; Washington State Univ., Pullman, WA (United States)

Nitrous oxide N₂O reduction is a big challenge due to high global warming potential of N₂O. (~300 times higher compared with CO₂). The best known catalysts, such as Rh/ceria, require relatively high temperatures for N₂O decomposition. Herein, we report that Ru/ceria catalysts with low Ru loading of ~0.25 wt% efficiently catalyze low temperature N₂O reduction by CO starting at 100 °C (full N₂O conversion below 200 °C) under industrially relevant flow rates and gas concentrations. Further, this remarkable performance stems from maintaining isolated Ru cations even on reduced ceria surface and, simultaneously, the propensity of Ru to affect ceria surface to form labile surface oxygen thereby creating large number of oxygen vacancies (Ce⁺³ cations) in the presence of CO. In contrast, for Rh/CeO₂ catalysts with equivalent metal loading, the activity is much lower because atomically dispersed Rh sinters into metallic clusters at the onset reaction temperature (~200 °C): these clusters are much less effective than isolated single Ru ions, with lower Ce⁺³ concentration maintained on reduced Rh/CeO₂ catalyst. Our study highlights the benefits of gaining molecular-level insight into the dynamic nature of catalytically active sites under reaction conditions for preparing catalysts containing low loading of precious metals with unsurpassed low temperature activity.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2395913

Report Number(s):: PNNL-SA--192651

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Vol. 343; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Co-existence of atomically dispersed Ru and Ce3+ sites is responsible for excellent low temperature N2O reduction activity of Ru/CeO2

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