Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 3, Issue 9, Pages 2435-2443Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cy00153a
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Funding
- National Basic Research Program of China [2011CB201405]
- National Natural Science Foundation of China [21203230]
- Natural Science Foundation of Shanxi Province [2012021005-5]
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A mesoporous Ni-CaO-ZrO2 catalyst which showed an excellent performance in the dry reforming of CH4 was thoroughly characterized by using a series of methods including N-2 physical adsorption, temperature-programmed reduction (TPR), H-2/CO chemisorptions, and so forth. Particularly, samples after different treatments such as calcination, reduction and different periods of reaction were subjected to X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analysis, by which changes in the phase structure and surface chemistry were followed. The results suggested that metallic Ni was gradually oxidized during the reaction, and a non-stoichiometric Ni-carbon compound was slowly formed. This latter species has a role as an important intermediate (or even active phase). Kinetic studies were then carried out based on these findings, according to which a Langmuir-Hinshelwood model was developed. Both the experimental results and the kinetic analysis provided novel evidence for the bi-functional mechanism of dry reforming over ZrO2-based catalysts.
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