Abstract
Different types of copper oxide in CuO–CeO2/Al2O3 were investigated structurally and catalytically. Standard preparation lead to the presence of CuO monocrystals and Ce1−xCuxO2−x as evidenced by XRD, HRTEM and EDX. Washing with nitric acid removed the monocrystals, while leaving the Ce1−xCuxO2−x solid solution. The Fourier transformed Cu K patterns for the HNO3-washed catalyst showed a diminished second Cu shell, characteristic for Ce1−xCuxO2−x as well as for X-ray amorphous nano-sized CuAl2O4 spinel phase. XANES analysis and first shell Cu fitting confirmed this CuAl2O4 like structure outside Ce1−xCuxO2−x. By modeling the Ce K EXAFS signal in the washed sample, the amount of Cu in Ce1−xCuxO2−x was determined to be 18 ± 6 %. Total oxidation of CO and C3H8 as model reactions showed little difference in activity between non-washed and washed CuO–CeO2/Al2O3, indicating that CuO monocrystals were hardly active at temperatures below 450 °C. XRD performed in situ during TPR and TPO showed that CeO2 in Ce1−xCuxO2−x added to the redox capacity of both CuO–CeO2/Al2O3 samples as it was partially reduced at 300 °C. At higher temperatures, the CuO monocrystals also participated in reaction, leading to a higher activity for the oxidation of CH4.
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Acknowledgments
This work was supported by the ‘Long Term Structural Methusalem Funding by the Flemish Government’, the IAP7/05 Interuniversity Attraction Poles Programme—Belgian State – Belgian Science Policy, and the Fund for Scientific Research Flanders (FWO-Vlaanderen) in supplying financing of beam time at the DUBBLE and SNBL beam lines of the ESRF and travel costs. The authors acknowledge support from G. Rampelberg with the XRD equipment, assistance from S. Nikitenko (XAS campaign 26-01-860) at DUBBLE, from O. Safonova and P. Abdala at SNBL (XAS campaigns 26-01-876 and 26-01-941) and from V. Briois for performing a test measurement on the washed CeCu-Al catalyst at SAMBA, SOLEIL synchrotron. The authors equally acknowledge support from Prof. C. Detavernier with the in situ XRD equipment (Department of Solid State Sciences, Ghent University).
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Galvita, V.V., Filez, M., Poelman, H. et al. The Role of Different Types of CuO in CuO–CeO2/Al2O3 for Total Oxidation. Catal Lett 144, 32–43 (2014). https://doi.org/10.1007/s10562-013-1144-x
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DOI: https://doi.org/10.1007/s10562-013-1144-x