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Highly Dispersed Copper Oxide Clusters as Active Species in Copper-Ceria Catalyst for Preferential Oxidation of Carbon Monoxide
Wang, WW; Du, PP; Zou, SH; He, HY; Wang, RX; Jin, Z; Shi, S; Huang, YY; Si, R; Song, QS; Jia, CJ; Yan, CH
2015
Source PublicationACS CATALYSIS
Volume5Issue:4Pages:2088—2099
Subtype期刊文献
AbstractCopper-ceria is one of the very active catalysts for the preferential oxidation of carbon monoxide (CO-PROX) reaction, which is also a typical system in which the complexity of copper chemistry is clearly exhibited. In the present manuscript, copper-ceria catalysts with different Cu contents up to 20 wt % supported on CeO2 nanorods were synthesized by a deposition-precipitation (DP) method. The as-prepared samples were characterized by various structural and textural detections including X-ray diffraction (XRD), Vis-Raman, transmission electron microscopy (TEM), ex situ/in situ X-ray absorption fine structure (XAFS), and temperature-programmed reduction by hydrogen (H-2-TPR). It has been confirmed that the highly dispersed copper oxide (CuOx) clusters, as well as the strong interaction of Cu-[O-x]-Ce structure, were the main copper species deposited onto the ceria surface. No separated copper phase was detected for both preoxidized and prereduced samples with the Cu contents up to 10 wt %. The fresh copper-ceria catalysts were pretreated in either O-2- or H-2-atmosphere and then tested for the CO-PROX reaction at a space velocity (SV) of 60 000 mL center dot h(-1.)g(cat)(-1). The prereduced 5 and 10 wt % Cu samples exhibited excellent catalytic performance with high CO conversions (>50%, up to 100%) and O-2 selectivities (>60%, up to 100%) within a wide temperature window of 80-140 degrees C. The in situ XAFS technique was carried out to monitor the structural evolution on the copper-ceria catalysts during the PROX experiments. The X-ray absorption near edge spectra (XANES) profiles, by the aid of linear combination analysis, identified the oxidized Cu(II) were the dominant copper species in both O-2- and H-2-pretreated samples after CO-PROX at 80 degrees C. Furthermore, the extended X-ray absorption fine structure (EXAFS) fitting results, together with the corresponding H-2-TPR data distinctly determined that the highly dispersed CuOx (x = 0.2-0.5) cluster, other than the Cu-[O-x]-Ce (x = 0.7-3.2) structure, were the crucial active species for the studied CO-PROX reaction.
KeywordSelective Co Oxidation Fuel-cell Applications Noble-metal Catalysts X-ray-absorption Water-gas Shift Low-temperature Cuo/ceo2 Catalysts In-situ Cuo-ceo2 Catalysts Redox Properties
Indexed BySCI
Language英语
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/24471
Collection中科院上海应用物理研究所2011-2019年
Recommended Citation
GB/T 7714
Wang, WW,Du, PP,Zou, SH,et al. Highly Dispersed Copper Oxide Clusters as Active Species in Copper-Ceria Catalyst for Preferential Oxidation of Carbon Monoxide[J]. ACS CATALYSIS,2015,5(4):2088—2099.
APA Wang, WW.,Du, PP.,Zou, SH.,He, HY.,Wang, RX.,...&Yan, CH.(2015).Highly Dispersed Copper Oxide Clusters as Active Species in Copper-Ceria Catalyst for Preferential Oxidation of Carbon Monoxide.ACS CATALYSIS,5(4),2088—2099.
MLA Wang, WW,et al."Highly Dispersed Copper Oxide Clusters as Active Species in Copper-Ceria Catalyst for Preferential Oxidation of Carbon Monoxide".ACS CATALYSIS 5.4(2015):2088—2099.
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