Synergistic catalysis of carbon monoxide oxidation over copper oxide supported on samaria-doped ceria

被引:136
作者
Wang, JB
Tsai, DH
Huang, TJ [1 ]
机构
[1] Natl Tsing Hua Univ, Dept Chem Engn, Hsinchu 300, Taiwan
[2] I Shou Univ, Dept Chem Engn, Kaohsiung 840, Taiwan
关键词
copper oxide; samaria-doped ceria; CO oxidation; synergism; surface lattice oxygen;
D O I
10.1006/jcat.2002.3580
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
Copper oxide supported on samaria-doped ceria (SDC) is chosen as a model catalyst for carbon monoxide oxidation to illustrate interfacial metal oxide-support interaction and synergism. The oxidation catalysis by CuO/SDC was studied to further elucidate the effect of oxygen vacancies on activity enhancement and light-off behavior. It was found that an approximate proportionality exists between the reducibility and the activity of catalysts. It is concluded that reducibility and susceptibility of change of oxidation states of copper oxides is key to catalytic activities, and the nonstoichiometric metastable copper oxide species formed during reduction are very active because of their superior capability to transport surface lattice oxygen. A preliminary mechanism involving surface lattice oxygen of CuO and oxygen vacancy participation is proposed to fully explicate the synergistic process leading to light-off. The cause of light-off is attributed to the formation of co-shared oxygen ions coupled with the creation of high-turnover-frequency active sites which are composed of metastable copper oxide species and oxygen vacancies of two types, V-o,V-CuO and V-o,V-SDC. Over these CuO/SDC catalysts, the active sites exhibit the Langmuir-Hinshelwood-type mechanism characteristic of precious metals although the redox-cycle mechanism is still operative. (C) 2002 Elsevier Science (USA).
引用
收藏
页码:370 / 380
页数:11
相关论文
共 51 条
[31]   Dynamic study of the oxidation state of copper in the course of carbon monoxide oxidation over powdered CuO and Cu2O [J].
Nagase, K ;
Zheng, Y ;
Kodama, Y ;
Kakuta, J .
JOURNAL OF CATALYSIS, 1999, 187 (01) :123-130
[32]  
PANAYOTO V, 1983, STUD SURF SCI CATAL, V75, P1449
[33]   COPPER OXIDE ON ALUMINA .I. XRD STUDIES OF CATALYST COMPOSITION DURING AIR OXIDATION OF CARBON MONOXIDE [J].
PIERRON, ED ;
RASHKIN, JA ;
ROTH, JF .
JOURNAL OF CATALYSIS, 1967, 9 (01) :38-&
[34]   VANADIUM-OXIDE MONOLAYER CATALYSTS .4. THE CATALYTIC-OXIDATION OF CARBON-MONOXIDE [J].
ROOZEBOOM, F ;
VANDILLEN, AJ ;
GEUS, JW ;
GELLINGS, PJ .
INDUSTRIAL & ENGINEERING CHEMISTRY PRODUCT RESEARCH AND DEVELOPMENT, 1981, 20 (02) :304-309
[36]   CATALYTIC REDUCTION OF NITROGEN OXIDE BY CARBON-MONOXIDE OVER METAL-OXIDE CATALYSTS - CORRELATION OF ACTIVITIES WITH SURFACE-STATES OF METAL-OXIDES [J].
SAKURAI, K ;
OKAMOTO, Y ;
IMANAKA, T ;
TERANISHI, S .
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 1976, 49 (07) :1732-1735
[37]  
SATTFIELD C, 1991, HETEROGENEOUS CATALY
[38]   REACTIVITY OF PTAL2O3 AND PT-CEO2AL2O3 CATALYSTS FOR THE OXIDATION OF CARBON-MONOXIDE BY OXYGEN .2. INFLUENCE OF THE PRETREATMENT STEP ON THE OXIDATION MECHANISM [J].
SERRE, C ;
GARIN, F ;
BELOT, G ;
MAIRE, G .
JOURNAL OF CATALYSIS, 1993, 141 (01) :9-20
[39]   Nature of copper active sites in the carbon monoxide oxidation on CuAl2O4 and CuCr2O4 spinel type catalysts [J].
Severino, F ;
Brito, JL ;
Laine, J ;
Fierro, JLG ;
Agudo, AL .
JOURNAL OF CATALYSIS, 1998, 177 (01) :82-95
[40]  
SHIH WH, 1995, THESIS NATL TSING HU