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

化学 催化作用 化学工程 离子 无机化学 工程类 有机化学
作者
Konstantin Khivantsev,Nicholas R. Jaegers,Hristiyan A. Aleksandrov,Inhak Song,Xavier Isidro Pereira Hernández,Mark Engelhard,Jinshu Tian,Linxiao Chen,Débora Motta Meira,Libor Kovařík,Georgi N. Vayssilov,Yong Wang,János Szanyi
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (9): 5029-5040 被引量:42
标识
DOI:10.1021/jacs.2c09873
摘要

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 NOx storage properties due to formation of stable Ru-NO complexes as well as a high spill-over rate of NOx onto CeO2. Only ∼0.05 wt % of Ru is required for excellent NOx storage. Ru1O5 sites exhibit much higher stability during calcination in air/steam up to 750 °C in contrast to RuO2 nanoparticles. 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.
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