EXAFS analysis of the L3 edge of Ce in CeO2:: effects of multielectron excitations and final-state mixed valence

被引:47
作者
Fonda, E
Andreatta, D
Colavita, PE
Vlaic, G
机构
[1] Univ Trieste, Dipartimento Sci Chim, I-34127 Trieste, Italy
[2] Sincrotrone Trieste SCpA, I-34012 Trieste, Italy
关键词
EXAFS; CeO2; multielectron excitations; final-state mixed valence;
D O I
10.1107/S0909049598010280
中图分类号
TH7 [仪器、仪表];
学科分类号
0804 ; 080401 ; 081102 ;
摘要
Cerium oxide (IV) (CeO2) is extensively employed in heterogeneous catalysis, particularly as a promoter of noble metal action in three-way catalysts. For this reason there is a great scientific and economical interest in the development of any possible chemical or structural analysis technique that could provide information on these systems. EXAFS spectroscopy has revealed itself as a powerful technique for structural characterization of such catalysts. Unfortunately good quality K-edge spectra of cerium are not yet easily obtainable because of the high photon energy required (>40 keV). On the other hand, at lower energies it is easy to collect very good spectra of the L-3 edge (5.5 keV), but L-3-edge spectra of cerium (IV) are characterized by the presence of two undesired additional phenomena that interfere with EXAFS analysis: final-state mixed-valence behaviour and intense multi-electron excitations. Here, a comparative analysis of the K, L-3, L-2 and L-1 edges of Ce in CeO2 has been made and a procedure for obtaining structural parameters from L-3-edge EXAFS, even in the presence of these features, has been developed. This procedure could allow further studies of catalytic compounds containing tetravalent cerium surrounded by oxygen ligands.
引用
收藏
页码:34 / 42
页数:9
相关论文
共 23 条
[1]   DIRECT USE OF X-RAY ABSORPTION NEAR-EDGE STRUCTURE TO PROVIDE EVIDENCE OF STATIC OR DYNAMIC ADMIXTURE OF 4F CONFIGURATIONS IN MIXED-VALENT MATERIALS [J].
BEAUREPAIRE, E ;
KAPPLER, JP ;
MALTERRE, D ;
KRILL, G .
EUROPHYSICS LETTERS, 1988, 5 (04) :369-374
[2]   SPECIFIC INTERMEDIATE-VALENCE STATE OF INSULATING 4F COMPOUNDS DETECTED BY L3 X-RAY ABSORPTION [J].
BIANCONI, A ;
MARCELLI, A ;
DEXPERT, H ;
KARNATAK, R ;
KOTANI, A ;
JO, T ;
PETIAU, J .
PHYSICAL REVIEW B, 1987, 35 (02) :806-812
[3]  
*CERN PROGR LIBR, 1992, REF MAN VERS 92 1
[4]   INFLUENCE OF DOUBLE-ELECTRON TRANSITIONS ON THE EXAFS L EDGES OF RARE-EARTH SYSTEMS [J].
CHABOY, J ;
MARCELLI, A ;
TYSON, TA .
PHYSICAL REVIEW B, 1994, 49 (17) :11652-11661
[5]   AN EXPERIMENTAL AND THEORETICAL-STUDY OF MULTIELECTRON EXCITATIONS AT THE L3 ABSORPTION-EDGE IN SOME RARE-EARTH ALLOYS AND THEIR HYDRIDES [J].
CHABOY, J ;
GARCIA, J ;
MARCELLI, A ;
RUIZLOPEZ, MF .
CHEMICAL PHYSICS LETTERS, 1990, 174 (05) :389-395
[6]   Multiple-edge EXAFS refinement: Short-range structure in liquid and crystalline Sn [J].
DiCicco, A .
PHYSICAL REVIEW B, 1996, 53 (10) :6174-6185
[7]   X-ray-absorption spectroscopy and n-body distribution functions in condensed matter .2. Data analysis and applications [J].
Filipponi, A ;
DiCicco, A .
PHYSICAL REVIEW B, 1995, 52 (21) :15135-15149
[8]   X-ray-absorption spectroscopy and n-body distribution functions in condensed matter .1. Theory [J].
Filipponi, A ;
DiCicco, A ;
Natoli, CR .
PHYSICAL REVIEW B, 1995, 52 (21) :15122-15134
[9]   RH-LOADED CEO2-ZRO2 SOLID-SOLUTIONS AS HIGHLY EFFICIENT OXYGEN EXCHANGERS - DEPENDENCE OF THE REDUCTION BEHAVIOR AND THE OXYGEN STORAGE CAPACITY ON THE STRUCTURAL-PROPERTIES [J].
FORNASIERO, P ;
DIMONTE, R ;
RAO, GR ;
KASPAR, J ;
MERIANI, S ;
TROVARELLI, A ;
GRAZIANI, M .
JOURNAL OF CATALYSIS, 1995, 151 (01) :168-177
[10]  
Kalos M. H., 1986, MONTE CARLO METHODS