Single Ru(II) Ions on Ceria as a Highly Active Catalyst for Abatement of NO

Khivantsev, Konstantin; Jaegers, Nicholas R.; Aleksandrov, Hristiyan A.; Song, Inhak; Pereira-Hernandez, Xavier Isidro; Engelhard, Mark H.; Tian, Jinshu; Chen, Linxiao; Motta Meira, Debora; Kovarik, Libor; Vayssilov, Georgi N.; Wang, Yong; Szanyi, János

doi:10.1021/jacs.2c09873

Single Ru(II) Ions on Ceria as a Highly Active Catalyst for Abatement of NO

Journal Article · Wed Feb 22 00:00:00 EST 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.2c09873· OSTI ID:1969016

^[1]; Jaegers, Nicholas R. ^[1]; ^[2]; Song, Inhak ^[1]; Pereira-Hernandez, Xavier Isidro ^[1]; ^[1]; Tian, Jinshu ^[1]; Chen, Linxiao ^[1]; ^[3]; Kovarik, Libor ^[1]; ^[2]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Institute for Integrated Catalysis
University of Sofia (Bulgaria)
University of Saskatchewan, Saskatoon, SK (Canada). Canadian Light Source, Inc.

Atom trapping leads to catalysts with atomically dispersed Ru₁O₅ sites on (100) facets of ceria, as identified by spectroscopy and DFT calculations. This is a new class of ceria-based materials with Ru properties drastically different from the known M/ceria materials. They show excellent activity in catalytic NO oxidation, a critical step that requires use of large loadings of expensive noble metals in diesel aftertreatment systems. Ru₁/CeO₂ is stable during continuous cycling, ramping, and cooling as well as the presence of moisture. Furthermore, Ru₁/CeO₂ shows very high NO_x storage properties due to formation of stable Ru–NO complexes as well as a high spill-over rate of NO_x onto CeO₂. Only ~0.05 wt % of Ru is required for excellent NO_x storage. Ru₁O₅ sites exhibit much higher stability during calcination in air/steam up to 750 °C in contrast to RuO₂ nanoparticles. Here we clarify the location of Ru(II) ions on the ceria surface and experimentally identify the mechanism of NO storage and oxidation using DFT calculations and in situ DRIFTS/mass spectroscopy. Moreover, we show excellent reactivity of Ru₁/CeO₂ for NO reduction by CO at low temperatures: only 0.1–0.5 wt % of Ru is sufficient to achieve high activity. Modulation-excitation in situ infrared and XPS measurements reveal the individual elementary steps of NO reduction by CO on an atomically dispersed Ru ceria catalyst, highlighting unique properties of Ru₁/CeO₂ and its propensity to form oxygen vacancies/Ce⁺³ sites that are critical for NO reduction, even at low Ru loadings. Our study highlights the applicability of novel ceria-based single-atom catalysts to NO and CO abatement.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: Bulgarian Ministry of Education and Science; Bulgarian National Science Fund; 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:: 1969016

Report Number(s):: PNNL-SA-181740

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 9 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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