Studies on the redox behaviour of La1.867Th0.100CuO4 and its catalytic performance for NO decomposition

Authors
Citation
Lz. Gao et Ct. Au, Studies on the redox behaviour of La1.867Th0.100CuO4 and its catalytic performance for NO decomposition, CATAL LETT, 65(1-3), 2000, pp. 91-98
Citations number
37
Categorie Soggetti
Physical Chemistry/Chemical Physics","Chemical Engineering
Journal title
CATALYSIS LETTERS
ISSN journal
1011372X → ACNP
Volume
65
Issue
1-3
Year of publication
2000
Pages
91 - 98
Database
ISI
SICI code
1011-372X(2000)65:1-3<91:SOTRBO>2.0.ZU;2-G
Abstract
La1.867Th0.100CuO4 was prepared by means of the citric acid complexing meth od. The reduction-oxidation (redox) properties of this composite oxide have been investigated by using the XRD, TGA, EPR, TPD, and SEM methods. The fr esh (non-reduced) La1.867Th0.100CuO4 catalyst is single phase with tetragon al K2NiF4-type structure. There were three reduction steps observed over La 1.867Th0.100CuO4 in the temperature ranges of 25-100, 100-300, and 300-500 degrees C, respectively. After reduction at 300 degrees C, the material sti ll retained its original single phase but there were oxygen vacancies gener ated in the lattice. After reduction at 500 degrees C, it decomposed to a m ixture of oxides. In the course of reduction, trapped electrons were genera ted. During the oxidation of the reduced sample, O-2(-) was detected. Appar ently, oxygen vacancies are able to stabilise O-2(-) on the surface of the -1ptcatalyst. NO adsorption on both the fresh and reduced La1.867Th0.100CuO 4 samples generated NO radicals and O-2(-) species. On a La1.867Th0.100CuO4 sample reduced at 300 degrees C, [O2NO2](2-) was generated in NO adsorptio n and decomposed to N-2 and O2- at ca. 730 degrees C. After reduction, the O2- inside the La1.867Th0.100CuO4 lattice became more mobile and participat ed in the decomposition of [O2NO2](2-). The fresh (non-reduced) La1.867Th0. 100CuO4 sample with cation defects in its lattice shows higher NO decomposi tion activity than the fresh La2CuO4 sample in which there are no cation de fects. The 300 degrees C-reduced La1.867Th0.100CuO4 with cation defects and oxygen vacancies is more active than the fresh one for NO decomposition. T he redox action between Cu+ and Cu2+ is an essential process for NO decompo sition.