期刊
ACS CATALYSIS
卷 10, 期 7, 页码 3968-3983出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b05486
关键词
CeO2; Fe doping; oxygen vacancy; DFT calculation; H2S-selective oxidation
资金
- National Key Research and Development Program of China [2018YFA0209304]
- National Science Fund for Distinguished Young Scholars of China [21825801]
- National Natural Science Foundation of China [21773030, 21603034, 21878052]
- Natural Science Foundation of Fujian Province [2017J05022]
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 CeO, with high durability. Among the synthesized catalysts, the one with well-defined (110) and (100) planes is highly active for H,S-selective oxidation with H2S conversion and sulfur selectivity of almost 100% at 220 degrees C, superior to most of the reported Cebased 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 H,S oxidation. The derived insights are important for the design of efficient ceria-related catalysts for practical applications.
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