Lattice defects and oxygen storage capacity of nanocrystalline ceria and ceria-zirconia

被引:518
作者
Mamontov, E
Egami, T
Brezny, R
Koranne, M
Tyagi, S
机构
[1] Univ Penn, Dept Mat Sci & Engn, Philadelphia, PA 19104 USA
[2] WR Grace & Co Conn, Grace Davison Res, Columbia, MD 21044 USA
[3] Drexel Univ, Dept Phys, Philadelphia, PA 19104 USA
关键词
D O I
10.1021/jp0023011
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
The atomic structures of nanocrystalline powders of ceria, CeO2, and ceria-zirconia solid solution, (Ce,Zr)O-2, were studied by the pulsed neutron diffraction technique. Ceria is used as an oxygen storage component in automotive exhaust emission control systems, but the degradation of its oxygen storage capacity (OSC) after extended use at high temperatures has been a problem. Our results for the first time establish a direct correlation between the concentration of vacancy-interstitial oxygen defects and OSC. The surface area, on the other hand, exhibits much less correlation with OSC. The results also show that zirconia, which is known to retard the degradation when incorporated into ceria, reduces ceria and preserves oxygen defects. It is suggested that oxygen defects are the source of OSC in ceria-based catalyst supports, and the preservation of oxygen defects is critical for the stability of OSC against thermal aging.
引用
收藏
页码:11110 / 11116
页数:7
相关论文
共 30 条
[1]   A STUDY OF THE DISORDER IN HEAVILY DOPED BA1-XLAXF2+X BY NEUTRON-SCATTERING, IONIC-CONDUCTIVITY AND SPECIFIC-HEAT MEASUREMENTS [J].
ANDERSEN, NH ;
CLAUSEN, KN ;
KJEMS, JK ;
SCHOONMAN, J .
JOURNAL OF PHYSICS C-SOLID STATE PHYSICS, 1986, 19 (14) :2377-2389
[2]   Computer simulation studies of bulk reduction and oxygen migration in CeO2-ZrO2 solid solutions [J].
Balducci, G ;
Kaspar, J ;
Fornasiero, P ;
Graziani, M ;
Islam, MS ;
Gale, JD .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (10) :1750-1753
[3]   CO oxidation for the characterization of reducibility in oxygen storage components of three-way automotive catalysts [J].
Bunluesin, T ;
Gorte, RJ ;
Graham, GW .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (1-2) :105-115
[4]   OXYGEN SPECIES ADSORBED ON CEO2-SIO2 SUPPORTED CATALYSTS [J].
CHE, M ;
KIBBLEWHITE, JF ;
TENCH, AJ .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS I, 1973, 69 (05) :857-863
[5]   DEFECT STRUCTURE OF CALCIUM FLUORIDE CONTAINING EXCESS ANIONS .1. BRAGG SCATTERING [J].
CHEETHAM, AK ;
FENDER, BEF ;
COOPER, MJ .
JOURNAL OF PHYSICS PART C SOLID STATE PHYSICS, 1971, 4 (18) :3107-&
[6]   Effect of ceria structure on oxygen migration for Rh/ceria catalysts [J].
Cordatos, H ;
Bunluesin, T ;
Stubenrauch, J ;
Vohs, JM ;
Gorte, RJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (02) :785-789
[7]   Energy-dispersive surface X-ray scattering study of thin ceria overlayer on zirconia: Structural evolution with temperature [J].
Dmowski, W ;
Mamontov, E ;
Egami, T ;
Putna, S ;
Gorte, R .
PHYSICA B, 1998, 248 :95-100
[8]  
DMOWSKI W, 1997, CERAM T, V73, P119
[9]   STRUCTURAL DEFECTS IN AMORPHOUS SOLIDS - A COMPUTER-SIMULATION STUDY [J].
EGAMI, T ;
MAEDA, K ;
VITEK, V .
PHILOSOPHICAL MAGAZINE A-PHYSICS OF CONDENSED MATTER STRUCTURE DEFECTS AND MECHANICAL PROPERTIES, 1980, 41 (06) :883-901
[10]  
EGAMI T, 1997, SAE J