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Highly Efficient Porous FexCe1–xO2−δ with Three-Dimensional Hierarchical Nanoflower Morphology for H2S‑Selective Oxidation
journal contribution
posted on 2020-03-12, 17:52 authored by Xiaohai ZhengXiaohai Zheng, Yanli Li, Yong Zheng, Lijuan Shen, Yihong Xiao, Yanning Cao, Yongfan Zhang, Chaktong Au, Lilong JiangCeO2-based
catalysts are potentially suitable for H2S-selective oxidation,
but their practical application is
limited due to the problem of sulfate formation. Herein, we report
a facile citric acid-assisted hydrothermal process for the fabrication
of porous Fe-doped CeO2 with flower-like morphology that
can drastically promote the catalytic activities of CeO2 with high durability. Among the synthesized catalysts, the one with
well-defined (110) and (100) planes is highly active for H2S-selective oxidation with H2S conversion and sulfur selectivity
of almost 100% at 220 °C, superior to most of the reported Ce-based
catalysts. Meanwhile, outstanding catalytic stability is achieved
because the presence of Fe ions alleviates ceria deactivation due
to sulfation. The results of systematic investigation prove that the
doping of Fe not only raises the density of oxygen vacancies but also
promotes the redox ability and oxygen activity of the catalyst. We
conducted in situ DRIFTS (diffuse reflection infrared
Fourier transform spectroscopy) experiments and density functional
theory (DFT) calculations to disclose the reaction mechanism of H2S oxidation. The derived insights are important for the design
of efficient ceria-related catalysts for practical applications.
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Keywords
ceria deactivationFe ionsdensityH 2 S-selective oxidationacid-assisted hydrothermal processH 2 S oxidationredox abilityFe-doped CeO 2reaction mechanismoxygen activitysulfate formationDFTsulfur selectivityceria-related catalystsH 2 S conversionCe-based catalystsDRIFTSoxygen vacanciesapplicationCeO 2flower-like morphologyThree-Dimensional Hierarchical Nanoflower Morphology
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