Developing Robust Ceria-Supported Catalysts for Catalytic NO Reduction and CO/Hydrocarbon Oxidation

Song, Inhak; Kovarik, Libor; Engelhard, Mark H.; Szanyi, János; Wang, Yong; Khivantsev, Konstantin

doi:10.1021/acscatal.4c04433

Developing Robust Ceria-Supported Catalysts for Catalytic NO Reduction and CO/Hydrocarbon Oxidation

Journal Article · Tue Nov 26 00:00:00 EST 2024 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.4c04433· OSTI ID:2564588

Song, Inhak ^[1]; Kovarik, Libor ^[1]; ^[1]; ^[1]; Wang, Yong ^[2]; ^[1]

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

Synthesis of robust and hydrothermally stable PGM/ceria materials for NO, CO, and hydrocarbon abatement remains a formidable challenge, as ceria and PGMs are known to sinter severely >800 °C under hydrothermal conditions, leading to irreversible activity loss. In this work, we tackle this challenge by synthesizing well-defined catalysts with atomically dispersed rhodium supported on ceria with varying abundance of (100), (101), and (111) facets. Evaluation of these catalysts for NO reduction by CO as well as CO and propylene oxidation under model and industrially relevant conditions reveals pronounced reactivity and stability differences. Different modes of interaction of Rh ions with the ceria facets and their facile reducibility were shown to be the crucial parameters controlling reactivity, resulting in pronounced activity and stability variations. Facet-dependent poisoning of surfaces by nitrites was identified as the main reason for deactivation of the catalysts at low temperature, which is mitigated for (111) ceria facets. (111)-enriched ceria nanoparticles survive very harsh hydrothermal aging at 950 °C by maintaining and preserving (111) facets, unlike other ceria nanoparticles which sinter into poorly defined shapes. Thus, putting atomically dispersed PGM sites on (111) ceria facets lead to the catalytic material with the highest activity and stability for all studied reactions, providing the pathway to catalysts that can endure extremely harsh hydrothermal aging conditions.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2564588

Report Number(s):: PNNL-SA--206078

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 24 Vol. 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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