Evolution of oxygen vacancies in MnOx-CeO2 mixed oxides for soot oxidation

被引:453
作者
Lin Xueting [1 ]
Li Shujun [1 ]
He Hui [1 ]
Wu Zeng [1 ]
Wu Junliang [1 ]
Chen Limin [1 ]
Ye Daiqi [1 ,2 ,3 ]
Fu Mingli [1 ,2 ,3 ]
机构
[1] South China Univ Technol, Sch Environm & Energy, Guangzhou 510006, Guangdong, Peoples R China
[2] Guangdong Prov Key Lab Atmospher Environm & Pollu, Guangzhou 510006, Guangdong, Peoples R China
[3] South China Univ Technol, Guangdong Prov Engn & Technol Res Ctr Environm Ri, Guangzhou 510006, Guangdong, Peoples R China
基金
中国国家自然科学基金;
关键词
MnOx-CeO2 mixed oxides; Soot; Solid solution; Oxygen vacancies; Surface active species; CATALYTIC COMBUSTION; DIESEL SOOT; SOLID-SOLUTIONS; LATTICE OXYGEN; CEO2; CATALYSTS; ACTIVE-SITES; NANOROD-LIKE; PART I; REDUCTION; ALUMINA;
D O I
10.1016/j.apcatb.2017.06.071
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxygen vacancy (O-vacancy) is essential in catalytic oxidation but little is known about its insight. Herein, a series of MnOx-CeO2 catalysts with various Mn/(Mn + Ce) molar ratios were synthesized with citric acid complex method for O-vacancy study in soot catalytic combustion. The samples were characterized by X-ray powder diffraction (XRD), N-2 adsorption/desorption, O-2-temperature programmed desorption (O-2-TPD), H-2-temperature programmed reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS) and in situ Raman spectroscopy. It has been shown that MnOx(0.4)-CeO2 catalyst presented more O-vacancies, thus exhibiting the highest catalytic activities and redox properties. With the utilization of in situ Raman, two types of O-vacancies, including Frenkel-type oxygen vacancy (F-OV) and intrinsic oxygen vacancy (I-OV), were clarified. Furthermore, the transform relation between F-OV and I-OV was found. Those two types of O-vacancies favored to the migration and transformation of active species, enhancing further the oxidation-reduction cycle and the catalytic activity for soot oxidation. In addition, Mn4+/Mn3+(Mn2+), O-latt, O-sur and Ce4+/Ce3+ were believed to play important roles in soot oxidation. Finally, evolution of O-vacancies was proposed, which is of significance for soot catalytic oxidation. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:91 / 102
页数:12
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