Influence of the oxidative/reductive treatments on the activity of Pt/Ce0.67Zr0.33O2 catalyst

被引:52
作者
Fan, J [1 ]
Wu, XD [1 ]
Ran, R [1 ]
Weng, DA [1 ]
机构
[1] Tsinghua Univ, Dept Mat Sci & Engn, Beijing 100084, Peoples R China
关键词
Pt; CeO2-ZrO2 mixed oxides; three-way catalysts; redox treatment; diffusion;
D O I
10.1016/j.apsusc.2004.10.006
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
A Pt/Ce0.67Zr0.33O2 powder catalyst was prepared by sol-gel method. The as-received sample was successively oxidized, reduced and re-oxidized. The samples were characterized by XRD, XPS, TPR and three-way catalytic activity evaluation. The results supported the re-organization of the support and the occurrence of a strong metal-support interaction (SMSI) effect between platinum and ceria zirconia mixed oxides. The oxidative/reductive atmosphere affected the structure and performance of the catalyst by the SMSI. It was suggested that a migration of Ce4+ from the bulk to the surface of the support took place during the reductive treatment, resulting in a formation of ceria-rich phase on the surface. The diffusion process was reversed when the atmosphere was switched to an oxidative one. The status of decoration or encapsulation of Pt by ceria-rich phase changed with the atmosphere, and hereby affected the activity of the catalyst. At temperatures below 300 degrees C, the re-oxidized sample exhibited the best activity while the reduced one behaved the worst on the conversion of NO and CO, and the as-received one showed the worst on the oxidation of HC. After then the activity of the four samples tends to be the similar. The surface and interfacial Pt-0 sites were both considered as the effective factors. Models were constructed to describe the diffusion of ions and oxygen vacancies as well as the possible surface structure serving as the carrier of Pt-0 site which impacted on the catalytic activity remarkably. (c) 2004 Elsevier B.V All rights reserved.
引用
收藏
页码:162 / 171
页数:10
相关论文
共 18 条
[11]   Preparation of ceria-zirconia sub-catalysts for automotive exhaust cleaning [J].
Masui, T ;
Ozaki, T ;
Machida, K ;
Adachi, G .
JOURNAL OF ALLOYS AND COMPOUNDS, 2000, 303 :49-55
[12]  
NELSON AE, 2003, APPL SURF SCI, V10, P212
[13]   Correlation between catalytic activity and support reducibility in the CO2 reforming of methane over Pt/CexZr1-xO2 catalysts [J].
Noronha, FB ;
Fendley, EC ;
Soares, RR ;
Alvarez, WE ;
Resasco, DE .
CHEMICAL ENGINEERING JOURNAL, 2001, 82 (1-3) :21-31
[14]   PHYSICOCHEMICAL PROPERTIES OF CE-CONTAINING 3-WAY CATALYSTS AND THE EFFECT OF CE ON CATALYST ACTIVITY [J].
NUNAN, JG ;
ROBOTA, HJ ;
COHN, MJ ;
BRADLEY, SA .
JOURNAL OF CATALYSIS, 1992, 133 (02) :309-324
[15]   Reactivity of Pt/ceria and Pt/alumina planar model catalysts prepared by colloidal lithography [J].
Österlund, L ;
Kielbassa, S ;
Werdinius, C ;
Kasemo, B .
JOURNAL OF CATALYSIS, 2003, 215 (01) :94-107
[16]   Role of cerium-zirconium mixed oxides as catalysts for car pollution: A short review [J].
Ozawa, M .
JOURNAL OF ALLOYS AND COMPOUNDS, 1998, 275 :886-890
[17]   The thermal stability and catalytic performance of Ce-Zr promoted Rh-Pd/γ-Al2O3 automotive catalysts [J].
Wu, XD ;
Xu, LH ;
Weng, D .
APPLIED SURFACE SCIENCE, 2004, 221 (1-4) :375-383
[18]  
Yu Yao Y., 1984, J CATAL, V87, P152