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Open AccessArticle

Pd4S/SiO2: A Sulfur-Tolerant Palladium Catalyst for Catalytic Complete Oxidation of Methane

1
Industrial Catalysis Institute, Laboratory Breeding Base of Green Chemistry-Synthesis Technology, Zhejiang University of Technology, Hangzhou 310014, China
2
Centre for Synthesis and Chemical Biology, UCD School of Chemistry, University College Dublin, Belfield, Dublin 4, Ireland
*
Authors to whom correspondence should be addressed.
Catalysts 2019, 9(5), 410; https://doi.org/10.3390/catal9050410
Received: 4 April 2019 / Revised: 29 April 2019 / Accepted: 29 April 2019 / Published: 30 April 2019
(This article belongs to the Special Issue Advanced Strategies for Catalyst Design)
Sulfur species (e.g. H2S or SO2) are the natural enemies of most metal catalysts, especially
palladium catalysts. The previously reported methods of improving sulfur-tolerance were to
effectively defer the deactivation of palladium catalysts, but could not prevent PdO and carrier
interaction between sulfur species. In this report, novel sulfur-tolerant SiO2 supported Pd4S
catalysts (5 wt. % Pd loading) were prepared by H2S–H2 aqueous bubble method and applied to
catalytic complete oxidation of methane. The catalysts were characterization by X-ray diffraction,
Transmission electron microscopy, X-ray photoelectron Spectroscopy, temperature-programmed
oxidation, and temperature-programmed desorption techniques under identical conditions. The
structural characterization revealed that Pd4S and metallic Pd0 were found on the surface of freshly
prepared catalysts. However, Pd4S remained stable while most of metallic Pd0 was converted to
PdO during the oxidation reaction. When coexisting with PdO, Pd4S not only protected PdO from
sulfur poisoning, but also determined the catalytic activity. Moreover, the content of Pd4S could be
adjusted by changing H2S concentration of H2S–H2 mixture. When H2S concentration was 7 %, the
Pd4S/SiO2 catalyst was effective in converting 96% of methane at the 400 °C and also exhibited
long-term stability in the presence of 200 ppm H2S. A Pd4S/SiO2 catalyst that possesses excellent
sulfur-tolerance, oxidation stability, and catalytic activity has been developed for catalytic
complete oxidation of methane. View Full-Text
Keywords: sulfur-tolerance; Pd4S; catalytic oxidation of methane; sulfur poisoning sulfur-tolerance; Pd4S; catalytic oxidation of methane; sulfur poisoning
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MDPI and ACS Style

Ma, L.; Yuan, S.; Jiang, T.; Zhu, X.; Lu, C.; Li, X. Pd4S/SiO2: A Sulfur-Tolerant Palladium Catalyst for Catalytic Complete Oxidation of Methane. Catalysts 2019, 9, 410.

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