Silicate-induced high-temperature-resistant small-crystallite ceria support enhancing palladium-catalyzed low-concentration methane combustion

[Display omitted] •Silicate-modified ceria crystallites have an average size of 6.7 nm at 800 °C.•Palladium catalyst supported on the modified ceria showed a significantly enhanced activity.•The small-crystallite ceria exhibited a high oxygen supply capacity.•The conversion of carbon-containing inte...

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Veröffentlicht in:Separation and purification technology 2025-01, Vol.353, p.128385, Article 128385
Hauptverfasser: Wu, Yang, Yang, Wenhu, Zhao, Ming, Xu, Haidi, Wang, Jianli, Chen, Yaoqiang
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Sprache:eng
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Zusammenfassung:[Display omitted] •Silicate-modified ceria crystallites have an average size of 6.7 nm at 800 °C.•Palladium catalyst supported on the modified ceria showed a significantly enhanced activity.•The small-crystallite ceria exhibited a high oxygen supply capacity.•The conversion of carbon-containing intermediates from methane dissociation on palladium species was enhanced. High-performance Pd/CeO2 catalysts for the purification of low-concentration methane in waste gases by catalytic combustion have long been pursued, given that methane is a potent greenhouse gas. The reduction in ceria oxygen supply and palladium dispersion, caused by ceria crystallite sintering, deactivates the catalyst. Here, we report an enhanced palladium catalyst supported on a silicate-induced small-crystallite ceria (7.2 nm) calcined at 800 °C, compared to the pristine ceria (50.7 nm). The catalyst was coated on a cordierite monolith for 0.1 vol% methane combustion, achieving 90 % methane conversion at 336 °C, which is 84 °C lower than the temperature required for Pd/CeO2 reference. The small-crystallite ceria exhibited a high oxygen supply capacity due to abundant oxygen vacancies, facilitating the conversion of carbon-containing intermediates from methane dissociation on palladium species, thereby enhancing the catalyst’s intrinsic activity. The catalyst, with increased palladium dispersion, demonstrated a methane reaction rate 6.7 times higher than that of the Pd/CeO2 at 280 °C. This study provides new insights into designing highly efficient Pd/CeO2-based catalysts for low-concentration methane combustion.
ISSN:1383-5866
DOI:10.1016/j.seppur.2024.128385