Journal
APPLIED CATALYSIS A-GENERAL
Volume 518, Issue -, Pages 87-101Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.apcata.2015.10.041
Keywords
Copper-ceria; Preferential oxidation of carbon monoxide; Ammonium carbonate leaching; X-ray absorption fine structure; Coprecipitation
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Funding
- National Science Foundation of China (NSFC) [21373259, 21301107, 11079005]
- Hundred Talents project of the Chinese Academy of Sciences
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA09030102]
- Fundamental research funding of Shandong University [2014JC005]
- Taishan Scholar project of Shandong Province (China), Open Funding from Beijing National Laboratory for Molecular Science
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Copper-ceria catalysts with the Cu contents up to 40 at.% were prepared by the coprecipitation method. Ammonium carbonate was used as the leaching agent on the as-calcined samples to remove the weakly bound copper species. The parent and leached catalysts were tested for the preferential oxidation of carbon monoxide (CO-PROX) reaction from 40 to 200 degrees C in 1%CO/1%O-2/50%H-2/N-2 with a space velocity of 60,000 mL h(-1) g(cat)(-1). When the Cu doping amount reached 30 at.%, the stable and constant CO-PROX reactivity, including CO conversion and 02 selectivity, was presented for both parent and ammonium carbonate leached catalysts. The fresh and used samples have been carefully characterized by various techniques such as power X-ray diffraction (XRD), X-ray absorption fine structure (XAFS), transmission electron microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS) and temperature-programmed reduction by hydrogen (H-2-TPR). It was confirmed that there are two different types of copper species, i.e. weakly bound CuOx clusters and strongly bound Cu-[O-x]-Ce structure, in both parent and leached catalysts. Furthermore, we have demonstrated that the weakly bound CuOx clusters removed by ammonium carbonate can be recovered by the migration of Cu-[O-x]-Ce species under the reduction or reaction conditions. The strongly bound copper species in CeO2 have been identified to be the reservoir for the active Cu sites for CO-PROX. (C) 2015 Elsevier B.V. All rights reserved.
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