期刊
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
卷 344, 期 1-2, 页码 28-36出版社
ELSEVIER
DOI: 10.1016/j.molcata.2011.04.018
关键词
CO2 reforming of CH4; Lanthanide promoter; Cobalt-nickel catalyst; Pauling electronegativity
资金
- Australian Research Council
- Australian Postgraduate Award
- University International Postgraduate Award
The influence of lanthanide group (Ce, Pr and Sm) promoters on alumina-supported bimetallic Co-Ni catalysts for CH4 dry reforming in a fixed-bed reactor was investigated. Lanthanide doping did not appear to affect CH4 and CO2 consumption rate, however, H-2 and CO production rates increased suggesting better utilisation of surface carbonaceous species. Carbon deposition on the promoted catalysts was substantially reduced (by up to 50%), with Ce providing the greatest anti-coking resistance followed by Pr and Sm. The beneficial effects of the promoted catalysts may be attributed to the interaction of the deposited but unconverted CxH1-x species with the lanthanide oxide in redox reactions, as well as smaller active particle size of the promoted catalysts which was unfavourable for carbon formation. In general, the study shows that attributes (such as product (H-2 and CO) formation rate constants and the associated reaction orders as well as the enthalpy and entropy of CH4 adsorption) of the promoted catalysts compared favourably to those of the unpromoted counterpart and are reasonably correlated with the Pauling electronegativity of the dopants. TPR-TPO of used catalysts suggests the presence two types of carbonaceous deposits - a reactive species which is lower in the promoted catalysts, and a relatively unreactive carbon which is present in similar quantities for all the catalysts. (C) 2011 Elsevier B.V. All rights reserved.
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