Enhanced CH4 and CO Oxidation over Ce1-xFexO2-δ Hybrid Catalysts by Tuning the Lattice Distortion and the State of Surface Iron Species

被引:83
作者
Li, Danyang [1 ,2 ]
Li, Kongzhai [1 ,2 ]
Xu, Ruidong [1 ]
Zhu, Xing [1 ,3 ]
Wei, Yonggang [1 ,3 ]
Tian, Dong [2 ]
Cheng, Xianming [1 ,3 ]
Wang, Hua [1 ,2 ,3 ]
机构
[1] Kunming Univ Sci & Technol, State Key Lab Complex Nonferrous Met Resources Cl, Kunming 650093, Yunnan, Peoples R China
[2] Kunming Univ Sci & Technol, Engn Res Ctr Met Energy Conservat & Emiss Reduct, Minist Educ, Kunming 650093, Yunnan, Peoples R China
[3] Kunming Univ Sci & Technol, Fac Met & Energy Engn, Kunming 650093, Yunnan, Peoples R China
基金
中国国家自然科学基金;
关键词
methane combustion; CO oxidation; structural dependence; Ce1-xFexO2-delta; catalysts; lattice distortion; IN-SITU; OXYGEN CARRIER; MIXED OXIDES; STRUCTURE DEPENDENCE; CEO2; NANOPARTICLES; RAMAN-SPECTROSCOPY; CRYSTAL PLANE; METHANE; COMBUSTION; SOOT;
D O I
10.1021/acsami.9b05409
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
CeO2-Fe2O3 mixed oxides are very attractive as catalysts for catalytic oxidation. Herein, we report the structural dependence of the Ce1-xFexO2-delta 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 degrees C) promotes the lattice distortion, whereas a lower temperature (0 degrees 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.
引用
收藏
页码:19227 / 19241
页数:15
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