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Highly Efficient Porous FexCe1–xO2−δ with Three-Dimensional Hierarchical Nanoflower Morphology for H2S-Selective Oxidation

  • Xiaohai Zheng
    Xiaohai Zheng
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
  • Yanli Li
    Yanli Li
    College of Chemistry, Fuzhou University, Fuzhou, Fujian 350116, P.R.China
    More by Yanli Li
  • Yong Zheng
    Yong Zheng
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    More by Yong Zheng
  • Lijuan Shen*
    Lijuan Shen
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    *Email: [email protected]
    More by Lijuan Shen
  • Yihong Xiao
    Yihong Xiao
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    More by Yihong Xiao
  • Yanning Cao
    Yanning Cao
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    More by Yanning Cao
  • Yongfan Zhang
    Yongfan Zhang
    College of Chemistry, Fuzhou University, Fuzhou, Fujian 350116, P.R.China
  • Chaktong Au
    Chaktong Au
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    More by Chaktong Au
  • , and 
  • Lilong Jiang*
    Lilong Jiang
    National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, P.R.China
    *Email: [email protected]
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Cite this: ACS Catal. 2020, 10, 7, 3968–3983
Publication Date (Web):March 3, 2020
https://doi.org/10.1021/acscatal.9b05486
Copyright © 2020 American Chemical Society
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Abstract

CeO2-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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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.9b05486.

  • Schematic of the system setup for H2S oxidation; peak shifts and cell parameters of CeO2 and xFeCe catalysts; O 1s XPS spectra of CeO2 and xFeCe catalysts; TEM image of 8FeCe and HRTEM image of CeO2; catalytic performance of reported Ce-based and Fe-based catalysts in H2S-selective oxidation; picture of sulfur collected from effluent; effect of SO2 and H2O on catalytic performance of the 8FeCe catalyst; amounts of H2 consumption and O2 uptake derived from H2-TPR and O2-TPD-MS; SEM image and mappings of the used 8FeCe catalyst; XPS O 1s spectra of fresh and used 8FeCe; DFT calculations of oxygen vacancy; O2, H2S, SH + H, and SO2 adsorption on the reduced pure and Fe-doped CeO2–x (110) surface (PDF)

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