期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 121, 期 -, 页码 65-74出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2012.03.022
关键词
Soot combustion; NOx reduction; Perovskite; Dual substitution; Mechanism
资金
- National Natural Science Foundation of China [21076146]
- Specialized Research Fund for the Doctoral Program of Higher Education of China [20090032110013]
- Program of New Century Excellent Talents in University of China [NCET-07-0599]
A series K/Cu simultaneously substituted nanometric perovskite catalysts La1-xKxCo1-yCuyO3-delta (x = 0, 0.1; y = 0, 0.05, 0.1, 0.2, 0.3) were synthesized by citric acid complexation, which were employed for soot combustion, NOx storage and simultaneous NOx-soot removal. The physico-chemical properties of the catalysts were characterized by XRD, FT-IR, EXAFS, SEM, H-2-TPR, Soot-TPR, TG/DTA, XPS and in situ DRIFTS techniques. When K and Cu are simultaneously introduced into LaCoO3, soot combustion is largely accelerated, decreasing the characteristic temperature (T-m) corresponding to the maximal soot combustion rate at least 80 degrees C; moreover, NOx reduction by soot is also remarkably facilitated. Among all the catalysts La0.9K0.1Co0.9Cu0.1O3-delta shows the lowest T-m of 360 degrees C, the highest NOx storage capacity (NSC) of 284 mu mol g(-1) and the largest NOx reduction percentage of 32%; for soot combustion, it also exhibits the lowest activation energy (80.04 kJ mol(-1)). The XPS and Soot-TPR results reveal that the catalyst La0.9K0.1Co0.9Cu0.1O3-delta possesses more active and larger amount of surface oxygen species (O-2(-) and O-), more tetravalent cobalt ions and better reducibility than others, which determines its better catalytic performance. Based on in situ DRIFTS and other characterization results, the potential mechanisms for soot combustion, NOx storage and simultaneous NOx-soot removal are proposed. (c) 2012 Elsevier B.V. All rights reserved.
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