Catalytic Activity and Reaction Mechanism of Ru-Modified Ce₀.₇Zr₀.₃Oₓ Catalysts for Selective Catalytic Oxidation of Ammonia

To solve the problem of the poor low-temperature NH₃ selective catalytic oxidation (NH₃–SCO) performance of CeZrOₓ catalysts, a series of Ru/CeZrOₓ catalysts with various Ru mass ratios were prepared via the impregnation–precipitation method. The introduction of Ru could significantly improve the lo...

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Veröffentlicht in:Energy & fuels 2024-11, Vol.38 (22 p.22440-22449), p.22440-22449
Hauptverfasser: Zhao, Hongzhe, Han, Zhitao, Cheng, Shaosi, Tian, You, Zeng, Qingliang, Li, Yeshan, Ma, Dong
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Sprache:eng
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Zusammenfassung:To solve the problem of the poor low-temperature NH₃ selective catalytic oxidation (NH₃–SCO) performance of CeZrOₓ catalysts, a series of Ru/CeZrOₓ catalysts with various Ru mass ratios were prepared via the impregnation–precipitation method. The introduction of Ru could significantly improve the low-temperature catalytic performance of CeZrOₓ catalysts from activity test results. Among prepared catalysts, the catalyst with a Ru mass ratio of 0.5 wt % and a Ce/Zr molar ratio of 7:3 (denoted as Ru₀.₅/CZO) was considered to have an excellent NH₃–SCO performance; NH₃ conversion reached 100 and 91.2% N₂ selectivity at 237 °C. Physicochemical properties of Ru₀.₅/CZO and CZO catalysts were compared through a series of characterization tests to investigate the relationship between the introduction of Ru and the NH₃–SCO performance. H₂-TPR results revealed an interaction between the Ru and Ce species. The introduction of Ru significantly shifted the reduction peak toward the lower-temperature direction, enhancing the low-temperature redox performance of the CZO catalyst. NH₃-TPD results indicated that Ru₀.₅/CZO catalysts had abundant acid sites on its surface, facilitating NH₃ adsorption and oxidation. In situ DRIFTS characterization results indicated that the reaction mechanism of the Ru₀.₅/CZO catalyst might be both internal-selective catalytic reduction (i-SCR) and imine (−NH) mechanisms.
ISSN:1520-5029
DOI:10.1021/acs.energyfuels.4c03739