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Enhanced CH4 and CO Oxidation over Ce1- xFe xO2-δ Hybrid Catalysts by Tuning the Lattice Distortion and the State of Surface Iron Species.

Danyang LiKongzhai LiRuidong XuXing ZhuYonggang WeiDong TianXianming ChengHua Wang
Published in: ACS applied materials & interfaces (2019)
CeO2-Fe2O3 mixed oxides are very attractive as catalysts for catalytic oxidation. Herein, we report the structural dependence of the Ce1- xFe xO2-δ catalysts for CH4 combustion and CO oxidation via changing lattice distortion degrees, surface Fe2O3 states, and oxygen vacancy concentrations. The lattice distortion degree and oxygen vacancy concentration of Ce-Fe-O solid solution can be tuned by changing the contents of Fe and the precipitation temperatures in the preparation process. The precipitation at relatively high temperature (70 °C) promotes the lattice distortion, whereas a lower temperature (0 °C) helps the formation of surface oxygen vacancies. The in situ diffuse reflectance infrared/Raman experiments and the physicochemical characterization suggest that both the CO and CH4 oxidations mainly follow a Mars-van Krevelen mechanism. Both the lattice distortion and the surface iron species play a crucial role in determining the catalytic activity by affecting the redox property of the catalysts. The surface iron species, combined with the oxygen vacancies, improve the catalytic performance by enhancing the adsorption capacity of reactants and reducibility of catalysts. The lattice distortion of CeO2 contributes to the catalytic activity by tuning the oxygen mobility in the bulk, which promotes the re-oxidation rate of catalysts.
Keyphrases
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